The footage shows the moment officers run to Mr Dos Santos’s car screaming, “Get out the car”, as a visibly distressed Mr Dos Santos shouts, “My kid is in the car.”
The footage was released by the police watchdog in connection with a police misconduct hearing into some of the officers involved in the stop on June 4 2020.
Mr Dos Santos and Ms Williams, both international athletes, believe they were racially profiled as they drove to their west London home from training with their then-three-month-old son in the back seat of their Mercedes.
The footage, released by the IOPC on Wednesday evening, shows the moment Mr Dos Santos, 28, who competed for Portugal in the 400m sprint at the Tokyo 2020 Olympics, was handcuffed and searched on suspicion of having drugs.
Ms Williams, 29, a gold medallist in the 4x100m relays at the 2018 European and Commonwealth Games, was also searched.
Nothing was found.
In the clip, officers can be heard claiming he was stopped because he had been avoiding police and that they could smell cannabis from the car, which he repeatedly denies.
Dashcam footage from the Met Police vehicle which followed Mr Dos Santos’ car was also released.
Earlier Wednesday, the athlete said he was not trying to “evade” the police or driving dangerously, and that he was “just trying to get home” because he feared for the safety of his family.
The misconduct hearing could see five officers sacked if allegations are proven.
Pc Casey, along with Acting Sergeant (A/PS) Rachel Simpson, Pc Jonathan Clapham, Pc Michael Bond and Pc Sam Franks deny all charges.
Mr Dos Santos told the hearing: “I didn’t want anything to happen to my family and I wanted to get home.
“I realised that the police carrier was following me and I hadn’t done anything wrong.
“I was afraid for the safety of Bianca and my son.”
When asked why he should be afraid of the police, Mr Dos Santos said he had “traumatic experiences” as a young black person who had been stopped by the police on “multiple occasions” in the past.
He added: “At that present moment my focus was the safety of Bianca and my son.
“I wanted to get home so they (the police) could see my other vehicles and know I wasn’t evading them.”
The five officers all face allegations that they breached police standards over equality and diversity during the stop-and-search.
A/PS Simpson and Pcs Clapham, Bond and Franks also face allegations that their actions amounted to a breach of professional behaviour standards in relation to the use of force.
They are said to have failed in relation to their levels of authority, respect and courtesy, as well as in their duties and responsibilities.
Pc Casey is also accused of breaching professional standards in the way he carried out his duties and responsibilities or gave orders and instructions.
It is also alleged that the honesty and integrity of Pcs Casey, Clapham, Bond and Franks breached professional behaviour standards.
The hearing continues.