Mr Goldsmith, who is also chief executive of Compass Pathways, said cash from a recent fund-raising round, which netted the company US$165m (NZ$234m), would be used to invest in the tie-up.
He said: "We want to bring relief and resilience to a huge number of people not helped right now by existing treatments and Covid has focused everyone's attention on just how important mental health is.
"One-third of patients with depression have treatment-resistant depression and what that cash does is enable us to advance our work in depression and look at other areas, such as anorexia, and areas of greatest unmet need where existing tools don't work well enough for enough people."
The substances in magic mushrooms have been used for hundreds of years and were rediscovered by Western medicine in the late 1950s.
Compass Pathways was founded after the couple's son was diagnosed with treatment-resistant depression and obsessive-compulsive disorder.
Mr Goldsmith said: "We did this for personal reasons when our son became ill.
"Katya [Ms Malievskaia] is a doctor and spent sleepless nights doing research and came across a small study treating OCD patients with psilocybin that was making a difference.
"She woke me up the next morning and said, 'you were alive in the Sixties and Seventies, what have you heard about magic mushrooms?' And that started us on a journey."
Compass's co-founders invested £1.5m (NZ$2.95m) in the business in its early days alongside three billionaire investors who put in £3m each.
The investors are Christian Angermayer, a German billionaire entrepreneur who, according to Mr Goldsmith "loves magic mushrooms"; Mike Novogratz, a hedge-fund billionaire and cryptocurrency investor; and Peter Thiel, the first external investor in Facebook and a co-founder of PayPal.
The trial sites are at King's College in London, Bristol, Manchester and Newcastle.
- Telegraph Media Group