Several MPs and families of gambling addicts who took their lives due to problem gambling participated in the walks, the fourth in a series of similar events since 2019.
The organisation pointed to Government statistics concerning gambling, with around 300,000 adults and 55,000 children in Britain considered to be problem gamblers.
The Big Step walks come amid the Government review of the 2005 Gambling Act, which has its deadline for evidence on 31 March.
Event organiser James Grimes said it aims to encourage people to contribute to the call for evidence, adding that more action must be taken from both the Government and the football industry.
"We are trying to amplify the voice of people with lived experience," said Grimes.
Around three-quarters of English Premier League clubs have betting sponsors or partners, with that total increasing to 87% for Championship clubs.
Over 7,000 people have signed a petition to end gambling sponsorship and advertising in football, with Grimes aiming to hand the petition to 10 Downing Street if it reaches 10,000 signatures.
