The pair were also the highest placed junior athletes for the second successive event and were only beaten by Olympians.
Samantha Murray, Olympic silver medallist from the 2012 London Games, won the women’s title, with Jamie Cooke triumphing in the men’s event.
In the women’s competition, Bryson impressed in the fencing, where she secured 20 victories, which put her in second place straight away.
She stayed in that position after the swimming, where she clocked 2:25.13, but Bryson had lost ground on former world champion Murray.
However, the Plymouth University medical student significantly cut that gap and crucially opened the one up between herself and the chasing pack with the quickest laser-run of the day.
Bryson, showing great consistency on the day, then finished the competition with the joint second-best ride to finish 60 points clear of third-placed Zoe Davison and only eight points behind Murray.
In the men’s competition, Pillage recorded 22 victories in the fencing to sit in third place after the opening discipline.
But he moved well into the lead after the swimming event, where he clocked 2:02.43, which was much faster than all his main rivals.
However, in the laser-run, Cooke made the decisive break at the end of the third loop to take a lead he would not relinquish. Pillage, though, stayed in the top two after edging out Tom Toolis on the final loop of the discipline.
The former Plymouth College pupil then produced an impressive ride to keep in silver medal position.
Both Bryson and Pillage will be part of the Great Britain team that will compete at the opening World Cup event in Egypt at the end of this month.
In the GB Youth Ranking event, Plymouth College’s Georgina Mitchell finished seventh and team-mate Annabel Denton ninth.