Tufts-bred roots-pop phenoms Guster have always had a nice-guys reputation. But even nice guys get fed up once in a while, and the band bring their pent-up frustrations to the fore on "Amsterdam," the first single from their second major-label album. "I threw away your greatest hits/You left them here the day you split," sings frontman Ryan Miller, who later in the song also rids himself of his departed friend’s bass guitar, vintage clothes, and drugs. He’s obviously a little bitter, but not enough to start thrashing away — the track’s driving beat and friendly guitar jangle are emblematic of the group’s best work.

On their previous album, Lost and Gone Forever (Warner Bros.), Guster made their pop ambitions apparent by working with veteran producer Steve Lillywhite and moving beyond their original acoustic-guitars-and-bongos configuration for the first time. This time they team up with producers Roger Moutenot and Ron Aniello to deliver a catchy adult-alternative disc that bears few traces of their jam-band beginnings. They’ve still got rhythm, but there’s a newfound maturity to both their arrangements and Miller’s lyrics. "Call your mom on the telephone/Tell her you’re coming home/Tell her there’s not a chance you’re ever gonna change the world," he sings over a jaunty psychedelic groove on "Red Oyster Cult"; the synth-flavored "Homecoming King" is just as melancholy.

Miller and guitarist Adam Gardner have some fun with their trademark vocal harmonies on the bluegrass ballad "Jesus on the Radio," and drummer Brian Rosenworcel is just as tasteful on a full kit as he was in the past on the bongos. The epic "Come Downstairs and Say Hello" unfolds with a looseness that verges on experimentalism: there’s a reason the band are working with long-time Yo La Tengo producer Moutenot. Guster are all grown up — and sounding better than ever.

(Guster perform next Tuesday, June 24 at City Hall Plaza; call 617-635-3911. They perform next Wednesday, June 25 at Monument Square in Portland; call 207-774-6364. And they perform next Thursday, June 26 at India Point Park in Providence; call 401-272-9550.)