Payet was one of the best players in the Premier League last season and has carried that form into the European Championship in France.
The 29-year-old attacking midfielder has been one of the best players for France in the tournament.
The former Marseille star has been linked with moves away from West Ham in the summer transfer window.
According to The Sun, Chelsea and Inter Milan are interested in signing Payet, while The London Evening Standard reported last month that West Ham fear that the attacker could force a move to Spanish giants Real Madrid this summer.
Comolli believes that West Ham should do all they can to retain the services of Payet for the 2016-17 campaign.
"You just have to see what is going in the transfer marker this summer to understand that prices are totally irrational so it is very difficult to put a price tag on a player,” Comolli told talkSPORT.
“But, if I was West Ham, I would do everything in my power to keep him because he was such a key element in their season.
"The talent has always been there. He just needed to click mentally, to understand what was needed to succeed at the top level and to make the best out of the fantastic skill he has got."
Payet has has scored three goals and created 21 chances in six matches for France at the 2016 European Championship so far.
The 29-year-old former Marseille star has a pass accuracy of 83% and a shot accuracy of 50%, and has won 15 dribbles and two tackles.
During the 2015-16 season, Payet scored nine goals and created 116 chances in 30 Premier League appearances for West Ham.