“Do you have any idea how crazy you are?” someone asks the indefatigable killer, Chigurh, in the Coen brothers’ infernal Texan thriller “No Country for Old Men.” Played by Javier Bardem, the black-clad seeker wears a serial murderer’s pageboy hairdo over a face that’s alternately mirthful and mirthless at all the worst times. Calm and methodical in planning and stride, he won’t stop till he finds the money, dogging his quarry like an angel of death.

Chigurh’s loot is plucked from the aftermath of a badlands drug shootout by amateur huntsman Llewelyn (Josh Brolin), an abler specimen of those Coen brothers creations who always try to get away with something. But that apocalyptic undertone radiates most from the movie’s deathly laconic source. Based on Cormac McCarthy’s 2005 novel, the Coens’ careful adaptation, which is the Centerpiece of the ongoing New York Film Festival, is a transfixing hellhound pursuit that’s insufficiently unified with intimations of moral decay from an aging sheriff.

Set in the wide-open Lone Star plains amid ordinary folk and dry boomerang wisdom (“I couldn’t swear to every detail … but it’s certainly a story”), “No Country” marks the fortuitous intersection of two major talents of pre-millennial America (the Coen brothers being one creative force). Admiration for both Mr. McCarthy and the Coens has long mingled with impatience with baroque stylings — heady, antiquarian, blood-tragedy prose for the novelist, and the brothers’ absurd pastiches and parodic grotesques.

But here the Coens latch on to the spareness of Mr. McCarthy’s novel and channel the energy of past excesses into a vaguely horror-movie craftsmanship of the chase, weighted by the tranquil, big-sky compositions of Roger Deakins’s cinematography. The feel, with streaks of wry and dark humor, evokes the shadowy suspense of the Coens’ first film, “Blood Simple,” and the regional austerity of their most acclaimed, “Fargo.”

Balancing the inhumanity of Chigurh and the human fallibility of Llewelyn is the middle-aged Sheriff Bell. He traces the wreckage of the single-minded pursuit (a strangled guard, bystanders put down with a boltgun), but often from a seated position. Stricken by the “signs and wonders” of the times, he chews over his young deputy’s reports more and more like a narrator, his face as careworn as the prairie is rugged. It’s his voice we hear first, ruminating, over an overture of landscape shots.

Chigurh, killing as he goes, toys with some of his victims, who make for a rural roll call: trailer park manager, gas station owner, motel clerks, border guard, a chicken farmer. With each encounter, and with exacting suspense crafted by the directors, Chigurh acts as a deadly visitation of fate with apparent impunity, keeping Llewelyn on the run. Played with loose affable stubbornness by Mr. Brolin, Llewelyn can only assure his wife (Kelly Macdonald) from afar, though she knows better and fears worse.

The dialogue is lively, as it always is in the Coens’ movies, though the wry stoicism, a shrewdness with a decent heart, flows originally from Mr. McCarthy’s pen. This coincidence turns out to be important in recognizing a weakness in the film’s integrity: Though both artistic voices painstakingly replicate Americana-steeped dialect, the Coens have rarely resisted a certain slippery irony and glibness that’s not always celebratory.

And sometimes, as we watch the oddly coiffed and impeccably wardrobed Chigurh come face to face with one of the credibly rough-hewn bit players, the uneasy disjunction threatens to spoil the salt-of-the-earth meditations that come from Sheriff Bell. The impending false note is heralded by the museum-like care given bloated corpses and scattered trucks, and sounded later by Llewelyn’s zany-biddie mother-in-law, who seems like something out of one the Coens’ less successful projects, “The Ladykillers.”

Aware of the need to match Mr. McCarthy’s tight moral structure, the Coens direct a Hitchcockian level of attention to visual motifs and eye-catching signposts — coins of fate, dogs, two boot tips spied under a tree. And Chigurh collides with the little worlds he razes: He’s the one who won’t play catch, tripping up or bulldozing the small talk that is the sturdy tool of quotidian virtue.

The little visual and verbal echoes help thread the clashing universes together, like when the same television reflects first Chigurh and, later in the movie, Sheriff Bell. But when Bell gravely relates his personal spiritual crisis and a feeling of being outmatched, a nagging sense of his separation from the rest of the film makes it hard for “No Country” to ascend as intended. It’s odd, then, that the Coens toss in a new, shapeless character (Woody Harrelson’s fixer) halfway through.

So “No Country for Old Men” is not a masterpiece, as many, starved of good Coen work, or maybe just competent celluloid menace, have claimed. But it’s a well-composed and deployed thriller with more than body counts on its mind, if perhaps more than it can convincingly express.