The development of advanced materials relies crucially on the availability of suitable high-resolution analytical characterization techniques. In this review, we discuss correlative microscopy methods combining Transmission Electron Microscopy (TEM) and Secondary Ion Mass Spectrometry (SIMS) for high-resolution high-sensitivity analysis. We review the literature on ex-situ TEM-SIMS correlation in materials science and beyond and motivate the need for in-situ TEM-SIMS. The instrument development aspects are discussed in detail followed by a computational analysis of the fundamental ion-solid interaction relevant for TEM-SIMS correlation. The correlative methodology and workflow are presented in detail together with a discussion on potential artifacts. Then, the strategies to enhance the performance characteristics such as the SIMS image resolution and sensitivities are discussed followed by example applications of the in-situ TEM-SIMS technique. Finally, the prospects of the TEM-SIMS correlative technique for solving challenging characterization problems are explored.