At the close, England had batted all day and were 318 without loss after winning the toss, with Cook unbeaten on 154 and Carberry, preferred as opener to Joe Root, on 153.
It is already the highest opening partnership at Hobart's Bellerive ground, and not since Graham Thorpe and Mark Ramprakash put on 377 against South Australia on the 1998/1999 tour have an England pair batted together for an entire day.
A dominant Cook conjured memories of his last triumphant Ashes tour of Australia three years ago with another big innings off 272 balls.
Carberry all but played his way into the Test team for the Ashes series opener against Australia in Brisbane on November 21 with his patient 288-ball innings, which included 22 boundaries and two sixes.
The 33-year-old Hampshire left-hander was given his chance to open with Cook after Root was bumped down to number five in the batting order for the Hobart game.
Carberry followed up his 78 in last weekend's drawn opening tour game against the WA Chairman's XI in Perth with another impressive audition for a Test spot.
He made his only Test appearance against Bangladesh in Chittagong in 2010, where he put on 72 and 65 batting with Cook at the top of the order.
Root appears to have paid the price for England's brittleness in the top order during the July-August Ashes series, when the home side failed to pass 400 in any of their innings.
On six occasions, England were three down for less than 65 runs and, aside from a big 180 at Lord's, Root struggled against Australian quicks Ryan Harris and Peter Siddle, who are likely to again have the new ball in Brisbane.
Australian leg-spin great Shane Warne said on Monday that Root would be "crucified" if he was picked to open in the Tests, and he is likely to find a place lower in the order as he averages 40 with two centuries from just 11 matches.
Cook, also criticised by Warne as a negative and unimaginative captain, showed glimpses of his best form in the 2010-11 Ashes in Australia, when he scored an unbeaten 235 and two other centuries.
England had an easy time against the thin Australia A bowling attack under sunny skies with just two recognised seamers in Trent Copeland and Ben Cutting, along with allrounder and captain Moises Henriques.
It was a deliberate tactic by Australia not to pick bowlers in Ashes contention for the Hobart match, however the plan might have backfired, with England's openers given an armchair ride into the coming Test series.
"Yeah possibly (a bowler short). We only had the five bowling options and with Moises being back from a long trip to India ... he didn't bowl as much as he would have liked to," Australia A wicketkeeper Tim Paine said.
"We didn't use the new ball as we could have ... we were a fraction short." Cook, batsman Kevin Pietersen, spinner Graeme Swann and paceman Stuart Broad were selected for their first outings on tour after all missed the Perth match.
Gary Ballance was included again after his first-ball duck in Perth as he bids to win the number six batting spot in the opening Ashes Test.