Sky Bet moved their price in from 12/1 to 6/4 in just half an hour as a wave of bets came in. Other firms in the industry made similar moves.
Former Chelsea star Poyet, currently in charge at Brighton, replaced Jose Mourinho as the market leader as a result of the gamble.
Sky Bet's Stuart Dallimore said: "We had several bets around the same time for Poyet to be the next Chelsea manager, most of which were to new accounts who were hitting their maximum.
"It's hard to say whether the money is from people who know or whether it's just a bit of a bandwagon punt.
"We're still wanting to keep Mourinho fairly short as that would be the choice for the fans and the person who Abramovich should appoint if he wants to win back some of the fans."
Current interim boss Rafael Benitez has shortened significantly in the Premier League 'sack race' market in recent days following the Blues' 2-2 FA Cup draw at League One Brentford on Sunday.
The former Liverpool manager was not a popular appointment with the club's fans back in November.
He has since won 10 of his 19 games in charge, although significantly Chelsea's home record under him is just three wins in eight.
A move for Poyet may prove popular with some supporters but his lack of experience as a manager at the highest level - he has yet to manage in the Premier League - would doubtless worry some.