We designed a novel, facile, and mass‐producible strategy for regulating the crystallizing and rheological behaviors of poly(butylene succinate) (PBS) by incorporating segmented PBS urethane ionomers (PBSUI). These macromolecular ionomers contain two segments: one is an ionic enriched segment, which can spontaneously form inter‐ and intramolecular ionic aggregates in PBS to serve as physical crosslinking points to increase the crystallization rate and complex viscosity of the PBS matrix; the other one is a PBS segment, which can improve the compatibility between the PBSUI and PBS matrix. The results from differential scanning calorimetry, polarized optical microscopy, dynamic mechanical analysis, and rotational rheometry suggest that the performance tunability of PBS was easily achieved by adding a very low content of PBSUI (1–5 wt %). PBS containing 3 wt % PBSUI, in which the mass ratio of ionic groups in PBSUI is 7.4%, showed the fastest overall crystallization rate at 12 times faster than PBS to finish crystallization, due to the remarkably increased nucleating efficiency. The dynamic mechanical analysis indicates that for those samples with relatively high ionic concentrations, a cluster of glass‐transition temperatures occurred that was related to an aggregation of PBSUI. The complex viscosity and storage modulus G′ of PBS/PBSUI were also increased, due to the ionic aggregates formed by PBSUI. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018, 135, 45545.