Transit-oriented development (TOD) has been regarded as an effective way to improve urban vibrancy and facilitate affordable, equitable, and livable communities in metro station areas (MSAs). Previous studies placed great attention on the interplay between the MSA-level built environment and overall human activities while neglecting the heterogeneity among different age groups. To address this gap, we leverage the mobile phone signaling data to quantify the spatio-temporal distribution of the MSA-level human activities among different age groups as measured by the vibrancy index (VI). Furthermore, we investigate the impact of the MSA-level built environment on the VI and its intergenerational differences by employing multiple linear regressions based on multi-sourced data. To this end, Chengdu—a TOD-thriving megacity in China—is chosen as a case study. The results indicate that: (1) Residential and bus stop density are positively associated with the VI. And the magnitudes of the correlation coefficients are similar among different age groups. (2) Distance to CBD is negatively associated with the VI of teenagers (12–18 years), middle-aged adults (40–59 years), and older adults (above 60 years) but unrelated to the VI of young adults (19–39 years). (3) Employment density is positively associated with the VI of young and middle-aged adults but insignificantly associated with the VI of teenagers and older adults. (4) The correlations between the floor area ratio and the VI are positive for all age groups. As age increases, the significance of such correlations becomes more pronounced. (5) Streetscape greenery shows a more significant positive correlation with the VI of teenagers and older adults as compared to those of young and middle-aged adults. (6) Significant negative correlations exist between housing price and the VI of different age groups. The findings can inform the development and design of vibrant TOD communities.