According to both the Center for Disease Control and the World Health Organization, contact transmission is the primary transmission route of infectious diseases worldwide. Usually, this is mitigated by a schedule of repeated regular sanitization, yet surfaces are easily recontaminated in the interim between cleanings. One solution to this problem is to generate self-disinfecting surfaces that can display sustained virucidal/antimicrobial properties against pathogens that settle upon them. Quaternary ammonium organosilicon compounds are ideal candidates to achieve this; cationic surfactants are safe and well-established surface disinfectants, while organosilanes are used broadly to form durable coatings with altered surface properties on many different materials. Despite their potential to circumvent the disadvantages of traditional disinfection methods, extant commercially available quaternary ammonium silanes do not display comparable efficacy to the standard surface disinfectants, nor have their respective coatings been demonstrated to meet the Environmental Protection Agency's guidelines for residual/extended efficacy. Inspired by the powerful surface activity of double-headed "gemini" surfactants, here, we present gemini-diquaternary silanes (GQs) with robust residual germicidal efficacy on various surfaces by incorporating a second cationic "head" to the structure of a conventional monoquaternary ammonium silane (MQ). Aqueous solutions of GQs were tested in suspension-and surface-antimicrobial assays against an array of pathogens, including Staphylococcus aureus, Escherichia coli, Pseudomonas aeruginosa, and severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). GQ performance was benchmarked against the common disinfectants, ethanol, hydrogen peroxide, hypochlorite, as well as MQ. Solutions of GQs were efficacious when used for immediate disinfection (>10 6 -fold reduction in 15 s). Additionally, GQs were demonstrated to impart durable self-disinfecting properties to a variety of porous and nonporous surfaces, effective after repeated cycles of abrasion and repeated contaminations, and with superior coating ability and activity (>10 8 higher activity) than that of MQs. GQs as surface treatments show great promise to overcome the limitations of traditional disinfectants in preventing the spread of infectious diseases.