Following a front-row lock-out of Barcelona's Circuit de Catalunya, Nico Rosberg and Lewis Hamilton hurtled backwards at an alarming rate in Sunday's Spanish Grand Prix.
Rosberg managed to claim sixth place, but finished 68 seconds behind race winner Fernando Alonso in his Ferrari.
Embarrassingly, Hamilton could not even hold on to a points-scoring position as he plummeted to 12th and was a lap down, coming home behind a Sauber and a Toro Rosso.
It was the starkest example yet of Mercedes' woes because it is clear they possess a strong car over one lap, but come race day it simply cannot look after its tyres.
A two-hour soul-searching debrief followed the race, but Mercedes appear to be some way from finding an answer.
"This car is a quick car," stated Wolff.
"I've been asked whether it has been made for a dragster race rather than a grand prix but no, it's something else.
"This is not about a team struggling with a car lacking pace, where you end up 15th on Saturday, and then 12th or 16th on Sunday.
"It is a car which is tremendously fast on Saturday, has real speed, but then on Sunday we are not able to manage the car with the tyres.
"It's something else which requires out-of-the-box thinking because this is a pattern we have seen in the past.
"Last season we saw a car that was good at the start of the season, that was a quick car, but performance deteriorated.
"So now it's about everybody in the team getting their heads together and analysing what we do from Saturday to Sunday, asking if there is anything we have not done until now.
"We need to try to question things we might not have questioned in the past.
"As I'm rather on the pessimistic side I don't believe in a magic golden key - I hope there could be.
"Instead it's about changing the approach, looking at the processes for racing."
Wolff is convinced there is no inherent car problem given it has taken the last three pole positions.
That is almost certain to be four in a row next up at Monaco, and given the narrow confines of the principality street circuit where overtaking is almost impossible, a win could be on the cards.
But a cautious Wolff said: "Monaco causes even more problems for us because we have always had a tendency of looking good there.
"It is so different to every other race track because you have no high-energy corners there, low grip.
"That means whatever we kick off (the car) now, the picture might be totally different in Monaco.
"It's very dangerous to have assumptions because in Monaco it either goes very well or not.
"Obviously, I'd love to win that one. We have two quick drivers, it's low grip, no high energy and we could be looking competitive, but I don't know."