It will be Frank's first-ever Champions League tie, and he's started well in his new position too, winning three of his four Premier League matches and looking good when doing so.
That will encourage the Spurs faithful, albeit Postecoglou also had a great start to his career at the Tottenham Hotspur Stadium before a second-season slide down the table.
Thomas Frank hasn't done well in Europe
Frank's only previous experience of European football with Brondby didn't go as well as might be expected, with three wins, three losses, and four draws in his 10 Europa League matches before moving to Brentford, so the 51-year-old will undoubtedly be looking to improve upon that.
LaLiga outfit Villarreal are the first to try their luck against the Lilywhites but history is against them. In 14 games against English sides in the premier European competition, the Yellow Submarine haven't won any (D6, L8).
Indeed, they've lost their last seven Champions League fixtures against teams from England with 57% of their losses coming against Premier League opposition.
They have, however, drawn both of the opening games of the competition when they've come up against English sides, thanks to goalless draws with Man Utd in 2005/06 and 2008/09.
It's also Villarreal's first foray into the UCL since 2021/22 when they made it all the way to the semi-finals, becoming the seventh Spanish top-flight side to do so after Barcelona, Valencia, Atletico Madrid, Real Madrid, Deportivo La Coruna and Real Sociedad.
First UCL campaign for Spurs since 2022/23
The 2022/23 campaign was the last time that the north Londoners were involved in the Champions League. Son Heung-min and Harry Kane - with 37 UCL goals between them for Spurs, making up 42% of their 89 goals in the competition since the rebranding - have now departed, meaning the likes of Brennan Johnson, Dominic Solanke (when fit again) and Richarlison have got to help write a new slice of Tottenham history in due course.
With just two goals in the competition, the Brazilian is the only current Spurs player with more than one UCL goal to his name, putting the squad's challenge into a little more perspective.
After already playing for Eintracht Frankfurt, Paris Saint-Germain and Juventus in the Champions League, Randal Kolo-Muani gets a chance to do so again with a fourth team in four seasons, a record for the competition. If he can recapture some of his early form, he too is likely to have a say in proceedings.
New signing Xavi Simons impressed against West Ham, as did former Hammer, Mo Kudus, and how well both start the game could be an indicator of just how well things will go on the night.
A night where, aside from Solanke, Frank will also be unable to call upon the services of James Maddison, Dejan Kulusevski, Yves Bissouma and Radu Dragusin.
Tottenham are notoriously slow starters
Notoriously slow starters in the UCL too, Tottenham have only won two of their opening games across seven previous editions of the competition, drawing two more and losing the other three.
Both of those wins were in north London, though, against Borussia Dortmund in 2017/18 (3-1) and against Marseille in 2022/23 (2-0).
Further, Spurs have only won one of their last 13 matches against teams from Spain, drawing five and losing seven, and it makes this first meeting between the sides in European competition the perfect opportunity for both teams to rewrite the script to an extent.
Villarreal's Juan Foyth, the youngest player to represent Spurs in the Champions League back in 2019 against APOEL, returns to north London, though Marcelino is likely to be without the injured Gerard Moreno, Logan Costa, Willy Kambwala and Pau Cabanes.
Villarreal need to reverse recent UCL history
If the visitors want to have any chance at reversing history for themselves, then Georgian striker, Georges Mikautadze, has to be involved at every opportunity.
Seven goals in eight starts in major European competition (four goals and three assists, all for Lyon in the Europa League last season) suggests that he will be the Submarine's standard bearer on the night.
A full-house is expected, and the magnitude of the occasion hasn't been lost on Thomas Frank.
"Obviously, it's a big thing. I am hugely looking forward to it," he said in his pre-match press conference. "I know it will be special when we have that Champions League anthem playing. That will be the moment. In front of our fantastic fans, it is a European night and we know they will be absolutely on it. It will be so special."
