SummarySorbent and functionalized polymers play a key role in a diverse set of fields, including chemical sensors, separation membranes, solid-phase extraction techniques, and chromatography. Sorbent polymers are critical to a number of sensor array or "electronic nose" systems. The responses of the sensors in the array give rise to patterns that can be used to distinguish one compound from another, provided that a sufficiently diverse set of sensing materials is present in the array. Figure S1 illustrates the concept of several sensors, each with a different sensor coating, giving rise to variable responses to an analyte that appear as a pattern in bar-graph format. Using hydrosilylation as the bond-forming reaction, we have developed a versatile and efficient approach to developing sorbent polymers with diverse interactive properties for sensor applications. Both the chemical and physical properties of these polymers are predictable and tunable by design.