To improve the accuracy of structural instantaneous frequency (IF) identified by the spline-kernelled chirplet transform, a combination of an improved spline-kernelled chirplet transform and a multi-synchrosqueezing technique is proposed for analyzing nonstationary signals and structural IF identification in this paper. Firstly, an improved spline-kernelled chirplet transform (ISCT) is put forward by introducing a three parameter Gaussian window function for an existing spline-kernelled chirplet transform. These three parameters are successfully obtained through an optimization algorithm and the energy concentration measure (CM). Then, combined with a multi-synchrosqueezing technique, a so-called improved multi-synchrosqueezing spline-kernelled chirplet transform (IMSSSCT) approach is further presented to improve the time–frequency energy concentration. Finally, the accuracy and practicability of the proposed IMSSSCT method are validated by analytical signals, a single-degree-of-freedom Duffing system, a three-layer shear frame, as well as a cantilever beam experiment. The research results indicate that the IMSSSCT technique can effectively and accurately identify the IFs of nonlinear and time-varying structures.