The mechanical properties of poly(butylene succinate) (PBS) were significantly enhanced by compounding cellulose‐acetate (CA) nanofibers (CA‐NF) to form CA/PBS composites. PBS has a great potential as an alternative material to other widely‐used polyolefins such as polyethylene and polypropylene made from petroleum. PBS is especially well‐known for its biodegradability, but the mechanical property of PBS was not sufficient as a commercial product for industrial applications. In this study, in order to enhance the mechanical property of PBS, a nanofiber made of CA was selected as a reinforcing material for the PBS composite. CA‐NF were successfully synthesized using the 20 wt % CA solution with acetone/N,N‐dimethylformamide (6/4 wt/wt) by electrospinning. The CA/PBS composites were then fabricated by mixing aligned or non‐aligned (random) CA‐NF. The highly oriented CA‐NF were obtained using a rotating collector at the rotating speed of 430 m/min. The cross‐sectional micrographs of the CA/PBS composites indicated that the electrospun CA‐NF had good compatibility with the PBS matrix. The mechanical properties of the CA/PBS composites were investigated by tensile testing. It was found that the Young's moduli of the composites with the aligned CA‐NF were higher than those of the composites with the random CA‐NF. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018, 135, 45429.