In the present work, heterogeneous multilayer ceramics based on two representative dielectrics, low-K Li2MoO4 (LM) and high-K [(Li0.5Bi0.5)(x)Bi-1-(x)][MoxV1-x]O-4 (LBMV), are successfully acquired using a convenient approach of self-constrained sintering at an ultralow temperature of 600 degrees C. These two materials with proximate but distinct sintering temperature ranges mutually act as constrained layers to each other in the process of densification, yielding significantly suppressed in-plane shrinkage of the LM/LBMV heterogeneous multilayer ceramics. Moreover, the dense heterostructures are endowed with decent mechanical and microwave dielectric properties. This work offers a new paradigm for facilely integrating heterogeneous dielectric materials for ultralow-temperature co-fired ceramics applications.