New Zealand-born Hartley has won 66 caps since his test debut in 2008. But he has also accumulated bans totalling 54 weeks for head-butting, biting, gouging, swearing at a referee, elbowing and punching, and was dropped from the squad for last year's Rugby World Cup.
Bookmaker William Hill also makes England, who face Wales and defending champions Ireland at home, 13/8 favourites to lift the trophy.
"We have seen a surge of bets for England to win both the Six Nations and the Grand Slam since Mr Hartley was confirmed as captain," said a spokesman for the bookmaker.
(Reporting by Simon Jennings in Bengaluru; editing by John Stonestreet)
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