In this paper, a low-temperature densification process of Al-Si alloy infiltration was developed to fabricate C/SiC-Ti3Si(Al)C-2, and then the microstructure, mechanical, and electromagnetic interference (EMI) shielding properties were studied compared with those of C/SiC-Ti3SiC2 and C/SiC-Si. The interbundle matrix of C/SiC-Ti3Si(Al)C-2 is mainly composed of Ti3Si(Al)C-2, which can bring various microdeformation mechanisms, high damage tolerance, and electrical conductivity, leading to the high effective volume fraction of loading fibers and electrical conductivity of C/SiC-Ti3Si(Al)C-2. Therefore, C/SiC-Ti3Si(Al)C-2 shows excellent bending strength of 556 MPa, fracture toughness 21.6 MPam(1/2), and EMI shielding effectiveness of 43.9 dB over the frequency of 8.2-12.4 GHz. Compared with C/SiC-Si and C/SiC-Ti3SiC2, both the improvement of mechanical properties and EMI shielding effectiveness can be obtained by the introduction of Ti3Si(Al)C-2 into C/SiC, revealing great potential as structural and functional materials.