Mainland Chinese grow up in a nation with Confucianism, Daoism and Buddhism as their cultural heritage, and are educated with atheism, materialism, and scientism in contemporary China. However, the high rate of conversion to Christianity among Chinese immigrants in Anglo-Saxon countries constitutes a distinctive feature in studies of migration. This paper aims to investigate the reasons for becoming Christian and the development of spirituality of a group of first-generation Chinese Australians from mainland China. All the seven participants are highly educated women who migrated to Australia as adults and had young children at the time of conversion. Data were collected mainly through open-ended in-depth interviews, and triangulated with private conversations, observations, and WeChat messaging. This ethnographic qualitative research found that these immigrants’ Christian attempts were prominently triggered by settlement crisis as new immigrants and as immigrant parents. They see Christianity and church community as a strong vehicle to resolve integration difficulties in a new society, such as economic and career insecurities, social isolation, language barriers, marital crises, and parenting dilemmas. Their Christian movement is facilitated by identified ideological congruence but hindered by cultural conflicts between their newly acquired Christian doctrines and their previously instructed values. The findings have implications for immigrant families, secular institutions, and religious organizations, as to the psychosocial well-being of new migrants.