Marcelino's over-achieving side are through to the last four of Spain's domestic Cup for the first time and showed when they twice took the lead at the Nou Camp in a La Liga game this month before losing 3-2 that they are not to be underestimated.
However, Barca, the record Cup winners, have clicked into something close to top form in recent weeks and Marcelino acknowledged Luis Enrique's men were playing some of their best football of the campaign.
Led by the fearsome attacking trio of Lionel Messi, Neymar and Luis Suarez, the Catalan giants are on a nine-match winning streak in all competitions and Marcelino called them an "extraordinary" team.
"We consider it a very tough challenge but that's not to say we are not going there with the ambition of getting a positive result," Marcelino told a news conference.
"Barca are the clear favourites because we are taking on the strongest Barca so far this season," he added.
"They have increased their attacking capabilities. Before their domination of possession was a given and now they have the resources to overcome their opponents depending on where they win back the ball.
"Their three forwards are worth seven or eight times Villarreal's annual budget. We will try to make sure it is not their day."
Villarreal spent a year in the second division in 2012-13 before bouncing back to qualify for the Europa League last term and are sixth in La Liga.
They have won plaudits for their entertaining style of play and will be seeking to avoid a result that turns next month's second leg at their Madrigal stadium into a lost cause.
"It's a very attractive tie for them, the first time in the Cup semi-finals," Barca coach Luis Enrique told a separate news conference.
"They are on a very good run and the match will have its difficulties, we know that from the La Liga game," he added.
The winners of the tie will play Athletic Bilbao, whose 23 Cup triumphs are bettered only by Barca's 26, or Espanyol in May's final.
Bilbao host Espanyol for their semi-final, first leg at the San Mames on Wednesday.
(Writing by Iain Rogers, editing by Justin Palmer)
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