We report large enhancement of upper critical field Hc2 observed in superconducting Sr2RuO4 thin films. Through dimensional crossover approaching two dimensions, Hc2 except the in-plane field direction is dramatically enhanced compared to bulks, following a definite relation distinct from bulk one between Hc2 and the transition temperature. The anomalous enhancement of Hc2 is highly suggestive of important changes of the superconducting properties, possibly accompanied with rotation of the triplet d-vector. Our findings will become a crucial step to further explore exotic properties by employing Sr2RuO4 thin films.