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Two types of new quaternary carbide solid solutions, (ZrC)[Al_<1-x>Si_x]_8C_6 with x=0.06 and (ZrC)[Al <1-y>Si_y]_4C_3 with y=0.04, have been synthesized and characterized using a laboratory X-ray powder diffraction (Cu Kα_1), transmission electron microscopy and energy dispersive X-ray spectroscopy (EDX). The average atom ratios [Al:Si] of both carbides were determined by EDX, and the crystal structures were refined using the Rietveld method. These carbides have been found to form a homologous series with the general formula (ZrC)_m[Al_<1-z>Si_z]_8C_6 (0?z?0.07), where m=1 and 2. The crystal structures can be regarded as intergrowth structures, consisting of the NaCl-type [Zr_mC_<m+1>] slabs separated by the Al_4C_3-type [Al_<1-z>Si_z)_8C_7] layers.