The 50-year-old is the longest-serving coach in Super League history but the Wolves, one of the pre-season favourites for the title, have struggled this year.
There is unlikely to be a shortage of suitors for the competition's longest-serving head coach, a two-times Super League victor with Leeds Rhinos, who took over at a low ebb at Warrington in March 2009 and steered the Wolves to three Challenge Cup victories and three beaten Grand Finals.
Warrington's fortunes changed drastically this season as they were consigned to the Qualifiers and, despite the team retaining their top-flight status with five wins from as many matches, Smith is set to move on.
It was a spectacular fall from grace after winning the League Leaders Shield past year and reaching both the Challenge Cup final and Grand Final.
Smith, who will stay in charge for those games, said: "I feel that it's now in the best interests of all of us to go in different directions".
'Unfortunately, things have not worked out this year but when people reflect back on his time here I'm sure they will do so with many fond memories.
"I'd like to think that while this has been a tough year, the club has progressed in the time I've been there in many ways, on and off the field, and is now in a position that means they can go on to bigger and greater things".
Owner Simon Moran said: "We would like to thank Tony for everything he has done for us".