Zoos in the 21st century are striving to make effective contributions to conservation. Although zoos are extremely popular and host over 600 million visitors worldwide, one challenge zoos face is how to effectively engage visitors and raise awareness and action for conservation. To this end, zoos commonly rely on charismatic megafauna, which have been shown to elicit a connection with zoo visitors. However, little is known about how to measure a connection to a species or how this connection may influence conservation behaviors. This study had two sequential objectives. The first was to develop a scale to measure visitors' connection to a species (Conservation Caring). The second was to investigate the relationship of Conservation Caring to pro-conservation behaviors, following a zoo experience. Pre- (n = 411) and post-visit (n = 452) responses were collected from three sites in order to assess the reliability and validity of a scale to measure Conservation Caring. Structural equation modeling was used to explore the relationship between Conservation Caring and pro-conservation behaviors. Conservation Caring was deemed a valid and reliable scale and was a strong predictor of species oriented behaviors (β = 0.62), for example, “adopting” an animal, but a weak predictor for biodiversity oriented behaviors (β = 0.07), for example, supporting sustainability policies. Results support the role zoos can play in fostering a connection to wildlife and stimulating pro-conservation behaviors. Additionally, visitors connected to a wide array of animals. On the basis of these results, zoos may recruit a wider assemblage of species as potential flagships. Zoo Biol. 32:528–540, 2013. © 2013 Wiley Periodicals Inc.