One thing is certain when you go to the Café Carlyle any time John Pizzarelli and Jessica Molaskey are co-starring. You are guaranteed top of the line musicianship, and that goes whether it is John on guitar, Jessica soloing, the two singing a duet or the spotlight shifting to their back-up musicians. Everything clicks smoothly, as unsurprisingly was the case on opening night of their latest gig (November 1-26, 2011) under the title “When Worlds Collide.”

Songs may collide in contrast, but the Pizzarelli-Molaskey togetherness as performers is as silky smooth and cool as ever. Thoroughly fine-tuned with each other, they engage in personable banter as well, with John carrying the bulk of the humor. It is all pleasantly low-key without the need to press too hard. Pizzarelli can get a laugh merely by introducing himself.

The program yielded much inventiveness in presentation. After getting us in the mood with “Walk Between Raindrops,” the couple launched into “Can’t Buy Me Love,” with musical references from “Wood Choppers Ball.” The combination of “Shine On Harvest Moon” by Norah Bayes and Jack Norworth and “Harvest Moon” by Neil Young also reflected the creative approach to choosing and juxtaposing material.

When it comes to getting the most out of a song, Molaskey can be terrific soloing. Her rendition of “In Buddy’s Eyes” by Stephen Sondheim, paired with “Rosalinda’s Eyes” by Billy Joel, was inspiringly beautiful. On the other hand, the couple can have fun speeding through tongue-twister lyrics with rhythmic intensity or reveling in a bit of scat.

Other highlights included doing justice to Paul Simon’s “Hearts and Bones” and “Gone at Last.” It fell to Pizzarelli to handle the encore chore, which he did with mellowness as he sang with mesmerizing tenderness “Our Love Is Here to Stay.”

The superb musical back-up, a major and integral part of the show, consists of Larry Fuller on piano, Martin Pizzarelli (yes, another one) on bass, and Tony Tedesco on drums.

You can’t have a better musical outing than catching Pizzarelli and Molaskey and their entourage at the Café Carlyle, Carlyle Hotel, Madison Avenue at 76th Street. Reservations: 212-744-1600.

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