The tour is part of yearlong celebrations marking the 400th anniversary of the King James Bible.
Premier Christian Radio presenter, the Rev Victor Robert Farrell, will preach from the 66 books of the Bible at each stop of the 66 city-tour over 66 days.
He set off from London on Sunday and will finish back in the capital on November 16 - 16/11, a reference to 1611, the year the King James Bible was completed.
Chris Knott Insurance has arranged and paid for the insurance to cover the tour car for the 3,300 mile journey which, in keeping with the theme, they were able to negotiate for £66.
Rev Farrell said: "What makes this tour so unique is that this is potentially the last year we'll have just 66 cities in the UK. The Queen can grant city status to any growing town and it is expected she will do so next year as part of her Diamond Jubilee celebrations."
"I'm really grateful to Chris Knott Insurance for agreeing to insure the tour car for us and for being so supportive of this mission to teach people about the God of the Bible, His plan and our lives as part of it."
Neil Franklin, managing director of Chris Knott Insurance said: "We're very interested in church and mission so how perfect that we could find cover for this unique 66-city bible tour for £66! We're delighted to be helping Robert on this worthwhile project".
On the web: www.66cities.org