In 1966 the GTO became a separate model line that included three body styles, the hardtop, coupe and convertible. Along with the separate identity for the GTO, it also took on a new totally new look. Overall the GTO was longer and heavier, even though, it still had the same 115 in wheelbase. Up front the split grille used vertical headlights, as before, but the grille openings tapered at the top and bottom as the grille approached the center dividing panel. The turn signal lamps were relocated next to the headlights and were attached to the new plastic grille. The hood, with its simulated scoop, was identical with the 1965, but now the Pontiac crest located on the front center.

The 1966 had a more distinct "Coke bottle" look. All 1966s used a thin side pinstripe, rocker panel moldings that continued along the bottom of the rear fenders and wheelwell moldings. GTO emblems were located in the same places as before: on the rear deck, on the rear fenders and on the grille. The GTO 6.5 liter crest was located on the front fenders behind the wheelwells. The rear was redesigned with a single taillight lamp unit and was covered by a housing with three horizontal louvers.

New for 1966 was the Custom wheel cover, which had twelve chrome and black spokes. The handsome Rally wheel was unchanged except that the center hubcap was painted flat-black around the lug nuts. The standard hubcap was a carry-over, as were the Deluxe wheel covers, but the minus the Pontiac Motor Division lettering. The wire wheel cover now incorporated a two-spoke spinner. All wheels measured 14 x 6 in., and 7.75 x 14 Red Line tires were once again standard, with whitewalls a no-cost option. This was the first year that the red fender liners were used. These were plastic shells molded to fit both front and rear wheelhouses and are considered a rare option.

The dash panel was redesigned, although, the familiar four-pod theme was still evident. Instrument and gauge selection was the same as in 1965. The instrument panel was covered with wood veneer. Optional on the standard panel were the Rally clock and the Safeguard speedometer. The Safeguard speedometer, which included a low-fuel warning lamp, allowed the driver to use a pointer to select a speed that when exceeded would sound a warning buzzer. If air conditioning was ordered the vent found above the heater and air conditioner controls on the 1965 GTOs was included on the 1966s only. A vinyl-trimmed assist bar was located above the glovebox door, with a GTO nameplate located to its left. The standard steering wheel was a two-spoke Deluxe unit, and the optional Custom Sports steering wheel was unchanged from 1965. Although bucket seats were standard equipment, an optional Strato Bench front seat was available.

The standard three-speed manual transmission came with a column-mounted shifter. Hurst shifters were standard equipment on the heavy-duty three-speed and four-speed manual boxes. The close-ratio four-speed was available only with 3.9:1 and 4.33:1 rear axle ratios. Engine availability was unchanged, with a 389 cid 335 hp V-8 standard and the 360 hp Tri-Power with a larger center carburetor still optional. During the model year, another engine option was released. This was known as the XS engine option, after its engine block code. It included the Air Scoop Package and a revised camshaft, and it was the first Ram Air engine. This option was available in 1965 but only as a over-the-counter or dealer installed option, now it could be ordered as a factory option The Air Scoop Package was also revised to accommodate the larger center carburetor. A compression ratio of 10.75:1 came on all engines.

A set of 9.5 in. drum brakes was still standard fare but now with metallic linings optional. An aluminum front drum option was part of the heavy-duty Ride and Handling Package. Exhaust splatters were not used; instead, chrome exhaust extensions exiting beneath the rear bumper were optional. All engines received 2 in Exhaust pipes and tailpipes. Production saw an all-time high in 1966. With totals reaching almost 100,000 units.

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