The 37-year-old Finn has looked very lively in the last two races, taking pole for Ferrari in Monaco last month, and brought his speed to Canada by clocking a time of one minute, 12.935 seconds around the 2.7 mile (4.34 km) Circuit Gilles Villeneuve, the only driver to dip under 1:13.00 on an overcast cloudy day.
Mercedes three-times world champion Lewis Hamilton was quickest in the morning session but could not match Raikkonen's pace in the afternoon, posting 1:13.150 ahead of arch-rival and championship leader Sebastian Vettel in the other Ferrari.
Vettel, a four-times world champion with Red Bull who leads Hamilton by 25 points after six races, was timed at 1:13.200 just in front of Mercedes' Valtteri Bottas on 1:13.310.
"The Ferraris are looking fast here and as the times show, it's super close at the top right now," said Hamilton.
"I feel like we are still just a little bit behind the red cars at this early stage of the weekend, but we'll be pushing as hard as we can to close the gap ahead of qualifying on Saturday.
"After a tough weekend in Monaco, the main thing is that our car is already feeling a lot better around Montreal.
"It should be game on for the rest of the weekend."
Young Dutchman Max Verstappen was fifth best in a Red Bull followed by veteran Brazilian Felipe Massa in a Williams.
MASTER HAMILTON
Hamilton, Vettel and Raikkonen have claimed wins in Montreal but the Briton is the master of the island circuit having collected five victories.
Putting a poor effort at the Monaco Grand Prix behind him, Hamilton, who can equal the 65 career pole positions of boyhood idol Ayrton Senna in Saturday's qualifying, has started from pole in Canada five times, including the last two years.
It was a day of adventure on the technical layout with driver after driver spinning off the track.
Vettel was off in both sessions, while Frenchman Romain Grosjean had his Haas spinning three times and Dane Daniil Kvyat twice.
It was another bitterly frustrating day for Fernando Alonso as the double world champion was forced to the sidelines in the morning session with mechanical problems then did not get back onto the track until late in the afternoon as his team struggled to fix hydraulic problems.
Alonso, who skipped the Monaco Grand Prix to race in the Indianapolis 500, has quickly discovered that little progress has been made at McLaren in his absence, leaving with a slim hope that his team can score their first points of the season.
Teenager Lance Stroll, the first Canadian in his home grand prix since Jacques Villeneuve in 2006, got his first test of the circuit, the Williams rookie recording the 13th best effort in the morning then slipping back to 17th in the afternoon.
(Editing by Mark Heinrich and Ken Ferris)
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