ZANDVOORT, September 14, 2013 (European Tour) - Jiménez followed his opening 64 with a blemish-free 67 at Kennemer, reaching nine under par for the week in the process.
He was joined late in the day by compatriot Larrazábal, with three-time winner Simon Dyson, his fellow Englishman Oliver Fisher and France’s Julien Quesne all one behind.
Dyson carded a seven under par 63 at Kennemer Golf Club, matching the course record held by himself and four other players at a venue where two of his three titles have come.
Jiménez, already the oldest winner in European Tour history after claiming the Hong Kong Open aged 48 and 318 days last November, had three birdies as he looks to claim his 20th European Tour title and 13th since turning 40.
"This course suits me," said the 49 year old, who won his second tournament in this event in 1994, albeit at a different course. "It's not a very long course but you have to have the ball in position.
"I like this kind of links course and I feel very comfortable with my game.
“I didn’t manage to get the win in Switzerland last week, but maybe this week it will be my turn - I hope so.”
Larrazábal was the only player able to overtake Jiménez when he played his first 12 holes in five under par, but a bogey at the 16th meant he had to settle for a 66 and a share of the lead.
The 30 year old, who has missed the cut in his last six events since finishing fourth in the Irish Open in June, said: "I'm happy, I'm hitting the ball as good as ever. I don't know how many putts I missed today on that back nine.
"But I am on top of the leaderboard at the moment, the conditions were not good this afternoon, it was raining all the way so I am very happy with my game."
As for playing with Jiménez, Larrazábal added: "It's always good, we spend many practice rounds together, maybe 95 per cent we play together. We know each other well and have a lot of fun. We have a lot of dinners together."
Dyson, whose victories at Kennemer in 2006 and 2009 both came in play-offs, carded seven birdies in a flawless round and his only dropped shots of the week so far came with a double-bogey six on his first hole of the opening round.
"I've done well in previous years and played well around it today," Dyson said. "I played really solid apart from the last two holes and never looked like making bogey.
"I hit a poor tee shot on the eighth, which was my 17th, and the lie determined the shot I had to play. I had quite a lot of room to pitch it on the green but had a terrible lie so had to play a little bump and run, a proper links shot, and managed to play it well.
"On the last I didn't quite strike the chip as I wanted to but it was nice to roll the putt in and have a bogey-free round."
Fisher celebrated his 25th birthday with a round of 65 to join Dyson and France's Julien Quesne on eight under par, with Scotland's David Drysdale seven under after a 64 featuring five birdies and an eagle.
Spain's Jorge Campillo was set to establish a new course record of 62 when he reached the 18th green eight under for the day, but a three-putt bogey meant he had to settle for a 63 and a share of seventh on six under.
Ryder Cup Captain Paul McGinley is just four off the lead after a birdie on the 18th meant he added a 67 to his opening 68, but three-time Major winner Padraig Harrington missed the cut after rounds of 71 and 69 left him level par.
Scores on Friday in the Dutch Open golf tournament at Zandvoort:
131 - Miguel Ángel Jimenez (ESP) 64-67, Pablo Larrazabal (ESP) 65-66
132 - Julien Quesne (FRA) 67-65, Simon Dyson (ENG) 69-63, Oliver Fisher (ENG) 67-65
133 - David Drysdale (SCO) 69-64
134 - Matthew Nixon (ENG) 69-65, Joost Luiten (NED) 69-65, Anthony Snobeck (FRA) 68-66, Jorge Campillo (ESP) 71-63
135 - Soren Kjeldsen (DEN) 68-67, Paul McGinley (IRL) 68-67, Damien McGrane (IRL) 65-70, Espen Kofstad (NOR) 69-66, Hennie Otto (RSA) 68-67, David Howell (ENG) 65-70, Simon Wakefield (ENG) 68-67, Michael Jonzon (SWE) 70-65, Gary Orr (SCO) 65-70
136 - Chris Paisley (ENG) 68-68, Andrew Marshall (ENG) 69-67, Brooks Koepka (USA) 70-66, Thomas Aiken (RSA) 72-64, Robert Allenby (AUS) 65-71, Richard Green (AUS) 70-66, Rafael Cabrera (ESP) 69-67, Álvaro Quirós (ESP) 72-64
137 - Jose María Olazabal (ESP) 69-68, Wu Ashun (CHN) 69-68, Alejandro Cañizares (ESP) 69-68, Felipe Aguilar (CHI) 69-68, Shane Lowry (IRL) 69-68, Grégory Havret (FRA) 67-70, Mikko Ilonen (FIN) 71-66, Prom Meesawat (THA) 67-70, Magnus Carlsson (SWE) 68-69, Rikard Karlberg (SWE) 70-67, Peter Hedblom (SWE) 71-66, Ross Fisher (ENG) 69-68, David Horsey (ENG) 71-66, Scott Jamieson (SCO) 69-68
138 - Richie Ramsay (SCO) 70-68, Scott Henry (SCO) 69-69, Robert Rock (ENG) 69-69, Chris Lloyd (ENG) 69-69, Mark Foster (ENG) 68-70, Paul Waring (ENG) 70-68, Richard Bland (ENG) 67-71, Tommy Fleetwood (ENG) 70-68, Richard Finch (ENG) 69-69, Björn Akesson (SWE) 71-67, Joakim Lagergren (SWE) 73-65, Darren Fichardt (RSA) 70-68, Fabrizio Zanotti (PAR) 65-73, Rowin Caron (NED) 73-65, Wil Besseling (NED) 67-71, Jeong Jin (KOR) 67-71, Mikko Korhonen (FIN) 71-67, Alexander Levy (FRA) 73-65, Simon Thornton (IRL) 70-68, Matteo Manassero (ITA) 70-68, Thomas Pieters (BEL) 68-70, Lasse Jensen (DEN) 72-66, Marcus Fraser (AUS) 67-71, Emiliano Grillo (ARG) 72-66
139 - Eduardo De La Riva (ESP) 68-71, Matteo Delpodio (ITA) 68-71, Lorenzo Gagli (ITA) 70-69, Alessandro Tadini (ITA) 72-67, David Higgins (IRL) 72-67, Kevin Phelan (IRL) 71-68, Christian Cévaër (FRA) 70-69, Ricardo Santos (POR) 70-69, Oscar Florén (SWE) 66-73, Seve Benson (ENG) 69-70, Paul Casey (ENG) 68-71, Matthew Baldwin (ENG) 69-70, Robert Coles (ENG) 69-70