Vaccine-laden baits were distributed to interrupt and halt raccoon (Procyon lotor) rabies transmission in suburban Nassau and Suffolk counties on Long Island, New York, US. Fishmeal polymer baits containing the RABORAL V-RG® vaccine were deployed with helicopters, bait stations, and vehicles at a target density of 250 baits/km2 during annual September campaigns (2006–10). Semiannual campaigns (500 baits/km2) were also initiated in a portion of the treatment zone (2007–09) in response to a persistent focus of rabid raccoons. The last enzootic case was reported in January 2009. The final vaccination campaign was completed in 2010. The raccoon variant of rabies virus is no longer circulating in Nassau or Suffolk counties. Significantly greater probabilities of raccoon seroconversion were observed in helicopter-deployed bait zones. The lowest probabilities of seroconversion were identified in vehicle and bait station-deployment bait zones, with a marginal advantage associated with bait-station deployment. Seroconversion was negatively associated with developed, medium-intensity areas and increasing human population density. Significantly higher rabies virus neutralizing antibody endpoint titrations were detected in helicopter and bait station-deployment zones.