Simeone, who made 11 appearances at three World Cups during his playing career, has seen Messi close up for Barcelona in recent seasons as coach of Atletico Madrid.
His Atletico side got the better of Messi and Barca this term to win La Liga but the 44-year-old feels the four-time FIFA Ballon d'Or winner can deliver the goods in Brazil.
Messi has struggled to consistently replicate his club form during two World Cup campaigns, playing eight times and scoring once as Argentina suffered quarter-final eliminations in 2006 and 2010 respectively.
However, Simeone claims pressure around his performance could help the captain and Argentina.
"After winning so much in Europe, it's normal that a World Cup could be tempting for him, that it could pose him extra responsibilities and pressures. But it'll be a great responsibility for him," he told Perform.
"There is no doubt that winning a World Cup makes you more special. Few players have had the chance to win it (from) our country. So that's why he and his team-mates will try to take Argentina to the best place in the world.
"It will be a unique opportunity in Brazil. They will have to compete well as a team, the way they have done recently. Alejandro (Sabella) has overseen this growth in the last stages of qualifying and also in recent friendlies.
"At the end of the day the progress must be shown on the pitch for all to see."
Simeone, who won two Copa America titles during his international career, also reiterated his desire to one day manage his nation after winning his fourth piece of silverware with Atleti this season.
"Of course I would like to coach Argentina one day but for now, I feel that I still want to coach from the touchline every day," he added.
"I look at the best national head coaches like Luis Aragones or Vicente del Bosque and I think you need to find the experience and wisdom you get from a long managerial career in order to be in the best seat in the world - your national side's.
"You need to be calm and patient and I'm not sure I have that right now due to my restlessness to be there on the pitch close to my players every day.
"Coaching a national side is different. That's why I'm convinced that you need a experience given by time and a patience given by the years to be in that place."
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