Negative thermal expansion (NTE) ceramics Sm 0.85 Zn 0.15 MnO 3 (SZMO) and ZrMgMo 3 O 12 (ZMMO) were selected to prepare Sm 0.85 Zn 0.15 MnO 3 -ZrMgMo 3 O 12 /Al-20Si (SZMO-ZMMO/Al-20Si) composites using ball milling and vacuum heating-press sintering processes in this study. The synergistic effect of the SZMO and ZMMO NTE ceramic reinforcements on the microstructure, mechanical properties, and coefficient of thermal expansion (CTE) of the composites was investigated. The results show that the processes of ball milling and sintering did not induce the decomposition of SZMO or ZMMO NTE ceramic reinforcements, nor did they promote a reaction between the Al-20Si matrix and SZMO or ZMMO NTE ceramic reinforcements. However, the excessive addition of SZMO and ZMMO NTE ceramics led to their aggregation within the composite. Adding a small amount of SZMO in combination with ZMMO effectively increased hardness and yield strength while reducing CTE in the Al-20Si alloy. The improvement in strength was primarily provided by SZMO, while the inhibition effect on CTE was primarily provided by ZMMO. An evaluation parameter denoted as α was proposed to evaluate the synergy effects of SZMO and ZMMO NTE ceramic reinforcements on the mechanical properties and CTE of the composites. Based on this parameter, among all composites fabricated, adding 2.5 vol% SZMO NTE ceramic and 10 vol% ZMMO NTE ceramic resulted in an optimal balance between CTE and strength for these composites with a compressive yield strength of 349.72 MPa and a CTE of 12.55 × 10 -6 /K, representing a significant increase in yield strength by 79.20% compared to that of Al-20Si alloy along with a notable reduction in CTE by 26.44%.