Previous studies demonstrated that methane can be used as an electron donor to microbially remove various oxidized contaminants in groundwater. Natural gas, which is more widely available and less expensive than purified methane, is potentially an alternative source of methane. However, natural gas commonly contains a considerable amount of ethane (C 2 H 6 ) and propane (C 3 H 8 ), in addition to methane. It is important that these gaseous alkanes are also utilized along with methane to avoid emissions. Here, we demonstrate that perchlorate (ClO 4 − ), a frequently reported contaminant in groundwater, can be microbially reduced to chloride (Cl − ) driven by C 2 H 6 or C 3 H 8 under oxygen-limiting conditions. Two independent membrane biofilm reactors (MBfRs) supplied with C 2 H 6 and C 3 H 8 , respectively, were operated in parallel to biologically reduce ClO 4 − . The continuous ClO 4 − removal during long-term MBfR operation combined with the concurrent C 2 H 6 /C 3 H 8 consumption and ClO 4 − reduction in batch tests confirms that ClO 4 − reduction was associated with C 2 H 6 or C 3 H 8 oxidation. Polyhydroxyalkanoates (PHAs) were synthesized in the presence of C 2 H 6 or C 3 H 8 and were subsequently utilized for supporting ClO 4 − bio-reduction in the absence of gaseous alkanes. Analysis by reverse transcription-quantitative polymerase chain reaction (RT-qPCR) showed that transcript abundance of bmoX (encoding alpha hydroxylase subunit of C 2 H 6 /C 3 H 8 monooxygenase) was positively correlated to the consumption rates of C 2 H 6 /C 3 H 8 , while pcrA (encoding a catalytic subunit of perchlorate reductase) was positively correlated to the consumption of ClO 4 − . High-throughput sequencing targeting 16S rRNA, bmoX, and pcrA indicated that Mycobacterium was the dominant microorganism oxidizing C 2 H 6 / C 3 H 8 , while Dechloromonas may be the major perchlorate-reducing bacterium in the biofilms. These findings shed light on microbial ClO 4 − reduction driven by C 2 H 6 and C 3 H 8 , facilitating the development of cost-effective strategies for ex situ groundwater remediation.