Spurs claimed only their second Premier League win under the arch and their first over the Reds since November 2012, with Harry Kane netting a brace and Heung-min Son and Dele Alli both scoring.
The Reds outfit could not live with Spurs' counter-attacking threat in the first-half, while the Lilywhites' third and fourth goals both came from set-pieces in front of a league-record crowd of 80,827.
The three points takes the North London side up to third, level on points with second-placed Manchester United, and five points off front-runners Manchester City.
Speaking to his post-match press conference afterwards, Pochettino hailed what he felt was an excellent display from all of his players.
Players deserve "big, big credit" for display
He said: "I'm so happy, very pleased. The effort was fantastic. I congratulate our players after Madrid to be ready again to compete in a big game.
"The way we started the game and how we played the first 45 minutes was very good. I am so pleased, for the team, for our fans because we've started to change the feeling that it was difficult to play here at Wembley.
"We've started to feel like it can be our home, and that is so important for the rest of the season to have that confidence."
Pochettino also declared that the result is another welcome one for his squad's morale, which was already high after earning a draw at Real Madrid in the Champions League on Tuesday.
"It's so important, that performance and that the dressing room has more confidence and more trust and we are working.
"I think it's so, so important. It's true that we are at the beginning of the season and many things can happen and it's a long way to the end but it's so important after a really good dressing room and performance in Madrid, that we won again against one of the best squads in the league.
"They're fantastic and the players deserve big, big credit for that."
Pochettino also revealed that his tactics in starting natural right-back Serge Aurier at left-back was to counter Mohamed Salah's pace.
"That is up to you," he said when asked by one journalist if his changes were deliberate or merely injury-enforced. "It was forced or not, I think when you decide to play in some way, sometimes it works, sometimes it doesn't.
"Of course, you always have some idea to play. Salah is a player that is played on the right with his left, always going inside and running and I think Serge is so fast and strong, he's right-footed and played in Toulouse and Paris Saint-Germain in that position.
"We won and we are so happy, but the credit is for the players that they play very well on the pitch."
"Kane one of the best players, not just strikers, in the world"
The Argentine was asked in particular about the sensational performance of goalscorer Kane, who proved a constant menace for the Liverpool defence and took his tally for the season to 13 goals in 12 games in all competitions.
"Another fantastic performance," enthused the Spurs manager in response. "He's amazing. One of the best players, strikers, in the world.
"But I'm happy with everyone because from the 'keeper - Hugo - to the front end, our strikers like Harry, they all gave their best and the performance was good.
"If you start to analyse, name by name, the team performance was very good.
"It was a very good game from both sides. Liverpool is a great team, great manager, they're always thinking to go forward, it's exciting, attacking football.
"I think they showed that, of course when you win you show it more but I think it was a fantastic afternoon to see a very good game."
Kane appeared to gesture that he felt a tweak in his hamstring after being brought off on 88 minutes, but Pochettino insists the problem was only fatigue.
"He was tired," he said. "He put in a massive effort at Bournemouth, Real Madrid and today and it's normal that he was a little bit tired. It will be no problem."
On the possibility of resting him for their League Cup clash with West Ham United in mid-week, Pochettino added: "Yes, maybe. We have many games, Wednesday and then Manchester United at the weekend, Real Madrid and then we finish against Crystal Palace.
"It's important to note that Harry played two games for the national team before Bournemouth. He's put in a massive effort, but he's performing that way because he's so professional.
"But he's not a machine and maybe Wednesday he needs to rest."