Arsenic and perchlorate are two types of emerging contaminants commonly found in various water bodies worldwide. Therefore, the development of effective removal technologies has become an important issue today. To this end, the following research studies were conducted. First, trimethylchlorosilane (TMCS) was used for the surface modification of a laboratory-prepared outside-in tubular TiO2/Al2O3 composite membrane aiming at enhancing the filtration performance of the said membrane layer. Second, the TMCS-modified tubular ceramic membrane coupled with the simultaneous electrocoagulation/ electrofiltration (EC/EF) process was tested and evaluated their combined performance in the remediation of arsenic- and perchlorate-spiked waters and one actual As-contaminated groundwater. In this research, the results of a preliminary electrocoagulation study have indicated that aluminum outperformed iron as the anode material. Thus, aluminum was selected as the sacrificial anode for the EC/EF tests throughout this work. In the course of various EC/EF testing, the removal efficiencies of the target contaminant in the test water specimens were compared for the tubular TiO2/Al2O3 composite membranes with and without surface modification. Also evaluated included the permeate flux, unit mass of target contaminant removed, and relevant power consumption. Though surface modification might not yield a better removal efficiency of the concerned contaminant, it gave rise to a greater permeate flux resulting in a greater removed mass of the contaminant for each of the synthetic wastewaters. Meanwhile, lower power consumption was found as compared with the case of no surface modification. As for the actual As-contaminated groundwater, the optimal EC/EF conditions for the tubular composite membrane without surface modification could low the As concentration to meet the local irrigation water quality criteria.