Despite the high availability of offline gambling in Macao, China, Internet gambling may remain attractive to many gamblers due to its anonymity and convenience. Given the scarcity of relevant research, this study aims to not only investigate the public attitude and prevalence of Internet gambling but also identify the demographic and psychological characteristics of Internet gamblers in Macao. We recruited 952 community adults with the random residential number dialing method and 427 university students through convenience sampling. Only 5.4% of the community adult respondents preferred online gambling compared to offline gambling, and the past-year prevalence of online gambling was about 1%. As hypothesized, Internet gambling was found to be positively associated with pathological gambling in both community and student samples. It was also associated with casino employment across samples. Moreover, we found that male gender, casino employment, materialism, and life dissatisfaction were significant risk factors of pathological gambling among Chinese gamblers. The findings provide insights on future designs of preventive measures and research direction for Internet gambling and pathological gambling in Chinese communities.