A significantly improved material is developed for application to chemiresistors, which are resistance‐based sensors for volatile organic compounds. This material is a polymer composite containing Au‐coated magnetic particles organized into electrically conducting pathways by magnetic fields. This improved material overcomes the various problems inherent to conventional carbon‐black chemiresistors, while achieving an unprecedented response magnitude. When exposed to chemical vapors, the polymer swells only slightly, yet this is amplified into large, reversible resistance changes, as much as (1 × 1011)% at a swelling of only 1.5%. These conductor–insulator transitions occur over such a narrow range of analyte vapor concentration that these devices can be described as chemical switches. The sensitivity and response range of these sensors can be tailored over a wide range by controlling the stress within the composite, including through the application of a magnetic field. Such tailorable sensors can be used to create sensor arrays that can accurately determine analyte concentration over a broad concentration range, or can be used to create logic circuits that signal a particular chemical environment. Polymer composites containing Au‐coated magnetic particles that are organized into electrically conducting pathways using magnetic fields are successfully used as chemiresistors. Absorption of chemical vapors elicits a reversible increase in the chemiresistor resistance. These sensors undergo a conductor–insulator transition over such a narrow concentration range that they can be described as chemical switches.