Remote sensing of solar-induced fluorescence (SIF) opens a new window for quantifying a key ecological variable, the terrestrial ecosystem gross primary production (GPP), because of the revealed strong SIF-GPP correlation. However, similar to many other remotely sensed metrics, SIF observations suffer from the sun-sensor geometry effects, which may have important impacts on the SIF-GPP relationship but remain poorly understood. Here we used remotely sensed SIF, globally distributed tower GPP data, and a mechanistic model to provide a systematic analysis. Our results reveal that leaf physiology, canopy structure, and sun-sensor geometries all affect the SIF-GPP relationship. In particular, we found that SIF observations in the sun-tracking hotspot direction can be a better proxy of GPP due to the similar responses of light use efficiency and SIF escaping probability in the hotspot direction to the increasing incoming solar radiation. Such conclusions are supported by a variety of modeling simulations and satellite observations over various plant function types, at different time scales and with satellite observational modes. This study demonstrates the potential and advantage of normalizing SIF observations to the hotspot direction for better global GPP estimations. This study also demonstrates the great potentials of current and future spaceborne sun-tracking satellite missions for a significant improvement in measuring and monitoring, at a wide range of spatial and temporal scales, the changes in terrestrial ecosystem GPP in response to anticipated changes in the Earth's environmental conditions.