Through Wynantskill, NY 66 becomes the main two-lane west/east street through the community, passing Evergreen Cemetery and a junction with the northern terminus of NY 150 (West Sand Lake Road). Remaining a two-lane commercial street, NY 66 continues west along Main Avenue along the Wyants Kill before leaving North Greenbush for the city of Troy. Upon entering Troy, NY 66 crosses the southern terminus of CR 142 (Mountain View Avenue). Passing through the Albia section of Troy, the route runs northwest along Pawling Avenue, remaining a two-lane residential street for a distance through Troy.