This paper addresses undergraduates' perception and behavioral intention (BI) toward Massive open online courses (MOOCs). It considers the moderating effect of culture to further explore the perceptions of students with different cultures to engage in MOOCs, providing MOOC suppliers with practical suggestions. 770 undergraduates in Spain and China are involved in this study. The proposed research model incorporating the technology acceptance model and theory of planned behavior is confirmed as a desirable theoretical model. Additionally, the moderating effect of culture has been confirmed between Spanish and Chinese students. The findings show Perceived usefulness and Perceived ease of use are effective in forming attitude (ATT). Besides, ATT and subjective norm, and perceived behavioral control are confirmed as vital factors impacting BI. Regarding the moderating effect of culture, significant differences have been detected to account for their behavior.