Ok, it was obviously close to going home time yesterday as I've just realised my question had nothing to do with SPServices! Just simple jQuery. After some more research I simply needed to add a : to the front of input:
$(":input[Title='DropDownColumnName']").val("ValueToSelect");
Not sure why, but this worked.
$(":input[Title='DropDownColumnName']").val("ValueToSelect");
Not sure why, but this worked.