At stumps on the second day at Kensington Oval, Australia had reached 44 without loss in reply with openers Ed Cowan on 27 and David Warner also unbeaten on 13.
Chanderpaul batted for 386 minutes for his unbeaten 103, becoming the leading run scorer in Tests at the Kensington Oval while skipper Darren Sammy thrilled the crowd with a quickfire 41.
"I never expected to be the person who had the most runs at Kensington. To have the most runs is a hell of an achievement," said Chanderpaul.
"Against an opposition like Australia if you're doing well against them you know the world is watching. When you go against them you have to bring your 'A' game. "You can't just walk out and decide that you can play anyhow against them. You have to step up." In the morning, Australia took the new ball as soon as it became available but it didn't seem to provide any more movement than the old one.
Skipper Michael Clarke had a gully and a short backward point in place to Darren Bravo and the plan worked when he played a tentative shot to the slower pace of Shane Watson, the ball going straight to Mike Hussey in the gully. Bravo's slow trudge off the field showed his clear disappointment after his innings of 51 had been brought to an end.
Narsingh Deonarine was playing his first Test for two years but, again, Australia had a clear plan. They served him up with the odd short ball and their preparation paid off. On 22, he was caught in two minds to a shorter delivery from Ryan Harris and as he turned away, the ball came off the edge and went high to wicket-keeper Matthew Wade who took his second catch.
After lunch, Carlton Baugh had moved on to 22 when he started off for an impossible single after Chanderpaul had turned the ball to square leg.
But Harris swooped and his direct hit dismissed the West Indies keeper.
This brought in Sammy and the West Indian captain was intent on attack. He had only been at the crease a few minutes when he smashed Nathan Lyon for three boundaries in four balls. He then ducked into a Watson delivery and needed several minutes of attention.
Next ball, still not fully recovered from the blow, Sammy powered the ball back over Watson's head for six. "I thought that was the right ball to bowl at that stage - bowling a good-length ball, but he seemed to enjoy it and hit it over my head. It was a good duel," said Watson.
"He took it very well and kept going. That's what you expect of an opposition skipper, to really dig in like he did and keep going through."
Both teams were showing aggression and the next few overs thrilled the crowd as the Australians goaded Sammy who hit back with another four and two more enormous sixes.
In the end, another short of a length ball from Ben Hilfenhaus saw him play uppishly to Cowan at square leg.
The West Indian skipper had hit 41 off just 36 balls; Chanderpaul only scored eight in their 53-run partnership.
Chanderpaul survived a close DRS decision on 85, the only one of the innings, when Lyon thought he'd trapped him lbw. Two balls later Lyon had his first wicket when skipper Clarke took a sharp catch at first slip but it was Kemar Roach on 16 that gave the chance.
With Chanderpaul on 95, Fidel Edwards threw away his wicket when he holed out a David Warner long hop to Mike Hussey.
Fortunately for the veteran West Indian, Devendra Bishoo was good enough to put on 28 for the next wicket to allow Chanderpaul to celebrate another century. West Indies are aiming for their first Test win against Australia for nine years and for a first series win over the visitors in 19 years.
