Davinson Sánchez’s 33rd-minute header put Spurs ahead before second half substitute Jamie Vardy missed a penalty with his first kick of the ball in the 60th minute.
Three minutes later, Christian Eriksen’s long-range effort beat Kasper Schmeichel in the Foxes’ net and, while Vardy did narrow the arrears with 14 minutes to play, Son Heung-Min struck in added time to seal all three points for Mauricio Pochettino’s title contenders.
City’s intent was evident early on as Maddison whipped a free-kick in for Harry Maguire to head towards goal, but home goalkeeper Hugo Lloris was able to tip it over the crossbar.
Academy graduate Barnes was the next Foxes man to go close in the ninth minute as he latched onto Tielemans’ insightful through-ball to fizz it across goal and narrowly wide.
Bittersweet Debut For Tielemans
Youri Tielemans was pleased to make his Leicester City debut at Tottenham but was left frustrated by the result.
Elsewhere, Schmeichel was called upon to make an instinctive point-blank save in the 18th minute when Danny Rose lashed it at goal, but the Dane was able to keep it out and the danger was cleared.
Just after the half-hour mark, Barnes was left to rue another missed chance to put Leicester ahead when Ben Chilwell slid him in behind the defence. His low drive, though, bobbled inches wide.
Two minutes later, Spurs were ahead. Eriksen cut inside his man and lofted a pin-point cross into City’s penalty area for Sánchez to nod beyond Schmeichel. 1-0 to the hosts.
Puel’s visitors continued their hunt for an equaliser and, on the stroke of half time, it almost came in remarkable circumstances as Tielemans looked for goal from the corner of the pitch.
The Belgian, with no other options around him, elected to half-volley it from the tightest of angles, forcing Lloris to scamper across his goal and send it behind for a corner-kick.
After the break, Llorente headed over for Spurs while Gray was twice denied by Lloris. It was quickly becoming an end-to-end affair, but one in which Leicester were in the ascendancy.
In the 60th minute, with Vardy about to join the action, Maddison was felled in the area by Jan Vertonghen, prompting referee Michael Oliver to point to the spot in front of the travelling supporters.
Vardy stepped up to take the spot-kick, aiming for the bottom corner, but France ‘keeper Lloris got down to make a firm save to stop Leicester from restoring a deserved parity on the scoresheet.
City were 2-0 down three minutes later. Spurs advanced in numbers and, when it fell to Eriksen on the edge of the area, the midfielder had time to pick his spot into the bottom corner.
Barnes was to be denied once again by Lloris within minutes of Tottenham’s second, as the 21-year-old was set free behind the defence, only to see another effort saved.
With 14 minutes to go, Leicester finally got a goal. Ricardo Pereira galloped down the right and played a low cross into Vardy, who duly obliged to poke it beyond Lloris from two yards out.
On 81 minutes, meanwhile, the 32-year-old received it from Ricardo again in the penalty area, before turning and shooting, but it agonisingly flew over Spurs' bar.
Kelechi Iheanacho, a late substitute, also missed a decent opportunity in similar circumstances for Puel’s side, while Chilwell twice forced Lloris into saving headers in quick succession.
With the Foxes pushing for a dramatic equaliser, Spurs broke one minute into added time and Son was left with an expanse of free space to run into before beating Schmeichel to wrap up the three points.
City's No.9 was unfortunate to find Lloris in such impressive form for the hosts.
When Jamie Vardy stepped up to take a penalty on the hour-mark, a successful spot-kick would have levelled the scores and swung momentum in Leicester's favour.
A fine stop from Hugo Lloris, though, maintained Spurs' advantage - which they doubled within minutes through Christian Eriksen - before ultimately condemning City to defeat.
City's newest recruit showed glimpses of his undoubted quality at Wembley.
Making his maiden appearance for the Foxes, Belgium international Youri Tielemans exhibited the reasons why the Club signed him on loan from AS Monaco on Deadline Day.
The 21-year-old was expressive for the visitors in London, often attempting to play in a team-mate in attacking positions, while showing the confidence to take his time and pick a pass.
Where do we stand?
City's forward players all had opportunities in the capital.
City sit 12th in the Premier League with nine wins and five draws from 26 matches, giving them a points tally of 32 and a goal difference of minus three.
Puel applauds the Foxes faithful at the full-time whistle.
Following a weekend of no football for the Foxes, Crystal Palace will visit King Power Stadium in the Premier League on Saturday 23 February (5:30pm GMT kick-off).
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