
The pair are set to play against their former club at Home Park on Saturday after regularly contributing goals and assists since joining the Pilgrims from the Valiants.
Tolaj was the first to make the move when Argyle activated a £1.1 million release clause in Tolaj's contract at Vale in August, which ended a long search over the summer for 'a number nine'.
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The Swiss striker has proved to be worth the wait with 20 goals in all competitions this season, 16 of them in League One, as well as seven assists.
Tolaj was followed to Argyle by another member of Vale's 2024/25 League Two promotion-winning squad when Curtis signed for the Pilgrims in January.
Generally used as a right-side attacking player, although he has had spells as a striker, Curtis has contributed seven assists and two goals, with his excellent deliveries at corners very productive for the Pilgrims.
However, had it not been for Argyle head coach Tom Cleverley and his staff watching Vale's first home game of the season, the 0-0 draw against Cardiff City on August 7, the pair might not have ended up at Home Park.
Cleverley said: "I always think recruitment is not luck, and why I say that is because we watch an incredible amount of football as a staff.
"We had eyes on the game that Vale played against Cardiff at home. They (Curtis and Tolaj) both played up top and I said 'They are my type of players'.
"You have to do the ground work. It's not all about data. Alright, data can help you in a 50-50 decision and make that decision a 60-40.
"That can help, but eyes on players, feet on the ground, is still a massive part of recruitment. Would we have had the two of them here unless I had really liked their performances that evening, I'm not sure?"
Tolaj has already played once against Vale, and scored a crucial goal as the Pilgrims beat them 1-0 at Vale Park in November to move above them and off the bottom of the table.
Vale went on to replace Darren Moore as their boss with Jon Brady at the start of January and although a 1-0 defeat at Cardiff City last night (Wednesday) confirmed their relegation back to League Two, they have shown considerable improvement.
While the Valiants were unable to retain their League One status they did make it all the way to the FA Cup quarter-finals, upsetting Bristol City and Sunderland along the way, before losing 7-0 to Chelsea at Stamford Bridge.
Argyle are still clinging to hopes of making the League One play-offs and Cleverley does expect their final home game of the regular season against Vale to be a straightforward one.
Cleverley said: "I tell you what does make it difficult is Port Vale have only lost four in their last 10. They have played Bolton, Huddersfield, Cardiff in that run.
"That's a resilient team, that's an organised team, a tough nut to crack and we fully understand that will be the challenge ahead of us.
"Okay, they got relegated last night but they look like they have got some good character in that dressing room and I don't think they will be taking their foot off the gas.
"Everyone has got something to play for at this stage of the season whether that's individually or collectively."
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