Horned Frogs linebacker Kenny Cain was equally impressive catching the ball.
Cain had two interceptions, returning one 40 yards to set up a field goal, and recovered a fumble after the first of Carter's two one-handed grabs. The Horned Frogs stretched their FBS-best winning streak to 11 in a row with 27-7 win over Virginia on Saturday.
"I never had a pick when I returned it. In high school I had two picks and I caught them and fell," said Cain, also a running back in high school. "Once I got the ball I realized my running back days were over."
Casey Pachall threw for 305 yards with three touchdowns and his first interception of the season for the Horned Frogs (3-0).
Pachall got a lot of help from Carter on the score that capped TCU's opening 94-yard drive after a punt that Virginia's Anthony Harris slapped back from the goal-line to prevent a touchback.
Carter was behind safety Brandon Phelps near midfield when he snared the pass with one hand, and then sprinted untouched to the end zone.
"I thought I put it a little high, but they have 6-7, 6-6 and 6-5 linemen who jump whenever you throw the ball," Pachall said. "I thought I got it over his head, but he made a great play. It's not that I expect it, but when it happens, it doesn't wow me because I've seen him do it numerous times, especially in practice."
Josh Boyce had his TCU-record 18th career touchdown catch. Freshman Jaden Oberkrom had field goals of 46 and 47 yards, the longer kick coming after Cain's long return.
Cain is the first TCU linebacker with two interceptions in a game since Chad Bayer on Nov. 20, 1999, the same day LaDainian Tomlinson set an NCAA record with 406 yards rushing for the Frogs against UTEP.
The Frogs hadn't allowed a touchdown this season until Virginia (2-2) finally scored with 4 1/2 minutes left, when backup quarterback Phillip Sims threw a 5-yard TD to E.J. Scott to make it 20-7.
"Even though the score is indicative of the way they played, believe it or not, there are some positive things that occurred for us against a top-20 team," Virginia coach Mike London said.
Carter had five catches for 128 yards, his second consecutive 100-yard receiving game. Pachall, the nation's most efficient passer, completed 21 of 32 passes and is the first TCU quarterback since Casey Printers in 2001 with consecutive 300-yard passing games.
Late in the first half, Carter reached up with his right hand for another big play, turning a short pass into a 43-yard gain to the Virginia 3.
"I usually don't try to catch it with one hand," Carter said. " The second one, I thought I was going to catch with both hands, but then my right hand just went out there and I caught it ... It's an instinct."
The Frogs failed to convert that one when Pachall tried to force a ball to Boyce that was intercepted by Maurice Canady, the first turnover Virginia forced this season.
Matthew Tucker, now the primary running back for TCU, ran 15 times for 52 yards. Leading rusher Waymon James is out for the season after a left knee injury, which he sustained in last week's 20-6 win at Kansas.
Boyce's TD catch put the Frogs up 14-0 in the second quarter. The play ended with Pachall emphatic fist-pumping and Boyce cradling the record-setting football to the sideline.
That seven-play drive was set up by Cain's fumble recovery at the Virginia 42. Kevin Parks, who had 84 yards on 12 carries, lost the ball after being hit by Elisha Olabode.
Cain's first interception came later in the second quarter on a ball that deflected off the intended receiver. In the second half on the pick he returned, Cain reached out and grabbed Michael Rocco's pass that was thrown behind a receiver.
TCU had two turnovers a week after four fumbles at Kansas in its first Big 12 league game. For the second game in a row, the Frogs had a fumble roll through the end zone to wipe away a likely score.
Skye Dawson had a 27-yard catch in the fourth quarter and was at the 2 when linebacker Daquan Romero hit him from behind, knocking loose the ball and through the end zone.
Darius Jennings had a long pass bounce off his facemask in the first half, and then late in the third quarter appeared to have a catch near the goal-line before a jarring hit by Chris Hackett knocked the ball loose for an incompletion.
But there were also the four turnovers.
"We drove the ball, had a lot of opportunities," said Rocco, who finished 13-of-28 for 126 yards. "But we kind of stubbed our toe on our own doing."