Spain's all-time top goalscorer Villa lifted La Liga, the Champions League and the Club World Cup in 2011 with Pep Guardiola's Barca as part of a fearsome front three alongside Messi and Pedro.
Debate has raged over whether the current 'MSN' trident should be considered the greatest ahead of the 2011 line-up or the attacking trio of Messi, Thierry Henry and Samuel Eto'o, who fired Barca to the treble in 2009.
But Villa has little doubt that Messi, Suarez and Neymar - who have inspired Luis Enrique's side to five trophies in 2015 - must be regarded as the finest forward line Camp Nou has seen.
"Without a doubt, it's the best trident in Barca's history," he said, as quoted by Sport. "It's undoubtedly the best.
"The numbers speak for themselves. You only have to analyse them: they're brutal, individually and collectively.
"I can say I was part of one of the best forward lines that the club has had."
Villa, now with MLS outfit New York City, praised the work of Luis Enrique in the past year following the pressure on his position 12 months ago.
"When he arrived, the team started with ups and downs, with criticism coming from everywhere and in the end Barca won everything again," the 34-year-old added.