Improving the logistics industry’s green total factor productivity (LGTFP) is a key source of power to achieve its high-quality development (HQD) in China. Technological innovation (TI) and environmental regulation (ER) policies are vital factors that affect the improvement of LGTFP. Although the impact of ERs or TI on LGTFP has been extensively researched, few studies have examined their combined effect. This study utilizes panel data from 30 Chinese provinces during 2006–2020 to estimate LGTFP using the Epsilon-based measure and global Malmquist–Luenberger index. Moreover, this study employs a dynamic spatial Durbin model to explore the influence of TI on LGTFP and its spatial spillovers, as well as the modulatory effect of ER in the relations between TI and LGTFP. The results show that (1) China’s LGTFP displays positive spatial spillovers and is influenced by the preceding period’s level. (2) In the short term, an improvement in TI levels had a positive effect on local LGTFP, but negative spillovers on neighboring districts. Nevertheless, in the long run, an improvement in TI levels had a notably negative influence on local LGTFP but positive spillovers on adjacent regions. (3) ER had an “inverted U-shaped” modulatory roles with spatial spillovers on the relations between TI and LGTFP in the long-term. These discoveries offer valuable insights into the coordinated development of TI systems and ER policies, enabling the formation of a policy system that aligns with the logistics industry’s HQD in China.