Smith reached his sixth Test century of the year and 13th overall with 134 and Voges remained unbeaten on 106 when the skipper declared Australia's first innings on 551 for three.
In reply the Caribbean tourists unravelled again and were 91 for six and trailing by 460 runs with three days left.
Hobart Test centurion Darren Bravo was on 13 with debutant Carlos Brathwaite three not out.
Smith called a halt to Australia's run plunder midway through the second day, while he was at the crease with Voges in an unbroken 223-run stand.
At the declaration he had scored 1,404 runs, ahead of Alastair Cook's 1,357 with England currently playing South Africa in Durban.
Voges also moved past 1,000 Test runs in his debut year with a total of 1,028 runs in his 18th Test innings.
Only two other batsmen have scored 1,000 or more Test runs in their debut year: Australia's Mark Taylor with 1,219 (1989) and Cook with 1,013 (2006).
Voges, who has yet to be dismissed in the series after scoring an unbeaten 269 in Hobart, lifted his average to an astonishing 542 in four Tests against the West Indies this year alone.
The Australians had four century-makers among their top five batsmen following Usman Khawaja's 144 and Joe Burns' 128 on Saturday's opening day. Only David Warner missed out with 23.
It was the first time that four Australian batsmen had
scored tons in a single Test innings in Australia.
The last time Australia had four centurions in an innings overseas was against England in Cardiff in 2009.
So far in the series, Australia have amassed 1,134 runs for the loss of just seven wickets against the wretched Caribbean tourists.
The Australians, who overpowered the Windies by an innings and 212 runs in the first Hobart Test, wasted no time slicing through the tourists' batting.
Kraigg Brathwaite was first to go, popping a catch to Burns at short leg off spinner Nathan Lyon for 17. His opening partner Rajendra Chandrika was leg before wicket without playing a shot to paceman James Pattinson for 25.
Senior batsman Marlon Samuels went lbw to Pattinson for a three-ball duck to continue his miserable series.
But Blackwood was out 10 balls later for 28, offering Lyon a return catch.
Denesh Ramdin swiftly followed, caught by Burns off Siddle for a duck, and skipper Jason Holder followed him the next ball -- bowled off-stump for a duck.
Carlos Brathwaite saw off the Siddle hat-trick attempt with a three down the ground.
Australia will retain the Frank Worrell trophy with victory against the struggling tourists, who last won a Test in Australia almost 18 years ago.
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