Why would two people over 21 have to pay a Licence bond in Wiltshire in the 1700s?
My 4x great grandparents paid a bond, even though they were both over 21.
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They would have to pay the bond if they broke the terms of that bond. A bond, whether that be a probate bond, bastardy bond, marriage bond, etc., is simply a legal instrument by which people swear to forfeit a certain sum if they do not carry out or comply with the terms of that bond.
Marriage bonds in the 1700s typically swore the groom and another one or two bondsmen to an oath that there was no legal impediment to marriage. This legal impediment might be that one or both of the parties were underage, they were related by a prohibited degree of consanguinity, or were already married. If the marriage was legal and there was no impediment, then they would never have paid the bond.
I suspect that your ancestors did not pay a bond, rather they paid for a marriage licence. Marriage bonds were one of the documents required when people married by licence. Marriage licences enabled people to marry with expediency, convenience, and privacy. The alternative was to publish banns in the parishes of both parties to be read on three Sundays. The reason bonds were required for marriage licences was simply that because there was not necessarily a public announcement of the marriage, the groom and bride had to be taken at their word that they were legally able to marry. The bond was a deterrent to proceeding with illegal marriages.