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The Ferrari driver and pre-event points leader improved on his form from FP1 by also leading the way in the second of Friday’s hour-long practice sessions in Barcelona.
Leclerc went clean on his soft Pirelli C3 tire qualifying run to a 1m 19.670s.
That was 0.16s better than his benchmark performance from FP1, plus just under 0.6s off Hamilton’s best time in the pre-season test at the venue in late February, which was set on the fastest C5 compound.
That put Leclerc 0.117s ahead of Russell, the Mercedes driver who set the pace in FP2 last time out for the inaugural Miami Grand Prix.
Hamilton was a late adopter of the soft tire and ran particularly well in the final part of the second sector to finish the third fastest performance – albeit a further 0.09s behind his teammate.
Meanwhile, before his home race, Carlos Sainz led the second Ferrari F1-75 to fourth place ahead of defending champion Max Verstappen.
Alexander Albon, Mick Schumacher, both Aston Martins and Esteban Ocon were the first drivers to take to the track in FP2 as the field initially stuck to the medium and hard compound tyres.
Sergio Perez and Albon also had their first run of the weekend after missing FP1 as Formula 2 race winner Juri Vips (Red Bull) and Formula E Champion Nyck de Vries (Williams) had their first GP weekend practice sessions performed.
Likewise, Zhou Guanyu returned to the Alfa Romeo cockpit after making way for Robert Kubica in practice one.
Verstappen was the first driver to set a fairly representative lap time on medium rubber as he and Sainz dropped below the 1:21 mark ahead of Leclerc and the Mercedes.
But after just 11 minutes, the session was interrupted by a virtual safety car.
This intervention was necessary when the Alfa Romeo of Valtteri Bottas, who was sixth at the time, ran out on the home straight after just three laps.
A puff of smoke from behind was accompanied by the engine, which appeared to promptly die as Bottas pulled to the edge of the track on the exit of Turn 1.
After the three minutes of the VSC, the other notable incidents happened to Albon and Lando Norris when both swerved wide to the right from the high-speed Turn 9.
So they had to look over the outer curb, kick up gravel and let sparks fly.
Both drivers expected damage to the ground of their FX machines but while Albon continued the session Norris was forced back into the McLaren garage for the remainder of FP2 after completing just six laps.
Albon and Sainz are also examined by the stewards after a close chat between the two at Turn 2.
After 21 minutes, the switch to soft tires and the Halo qualifying runs, Vettel came out on top with the heavily updated and controversial Aston Martin AMR22.
His 1’20.703 – fastest at the time at 0.23s – was soon eclipsed by Perez, although the Red Bull driver lost some pace due to traffic at Turn 10.
Verstappen then buzzed the timeline with his 1m20.006s, finding a huge 0.7s advantage at that point.
He remained the fastest rider in the first and last sectors but fell back in the middle part of the lap.
Then Sainz, the Mercedes and Leclerc set the ultimate times to lead FP2.
Things were less rosy for Leclerc in his late race on mid-size tires as he lost several tenths a lap on Verstappen when he complained about tire behavior and degradation.
Fernando Alonso led his Alpine to sixth in front of his home crowd, while Perez and Vettel slipped to seventh and eighth, ahead of Esteban Ocon and Mick Schumacher.
Pierre Gasly was the first driver to miss the top 10, the AlphaTauri overtaking Kevin Magnussen and Lance Stroll’s Haas.
Yuki Tsunoda finished 14th ahead of Daniel Ricciardo to end a busy afternoon for McLaren, while Bottas’ very early dip left him in 16th ahead of stablemate Zhou.
Norris rounded out the times behind the two Williams, Albon passed Nicholas Latifi.
