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The quantum spin liquid candidate <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mi>κ</mi></semantics></math></inline-formula>-(BEDT-TTF)<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>2</mn></msub></semantics></math></inline-formula>Cu<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>2</mn></msub></semantics></math></inline-formula>(CN)<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>3</mn></msub></semantics></math></inline-formula> has been established as the prime example of a genuine Mott insulator that can be tuned across the first-order insulator–metal transition either by chemical substitution or by physical pressure. Here, we explore the superconducting state that occurs at low temperatures, when both methods are combined, i.e., when <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mi>κ</mi></semantics></math></inline-formula>-[(BEDT-TTF)<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mrow><mn>1</mn><mo>−</mo><mi>x</mi></mrow></msub></semantics></math></inline-formula>(BEDT-STF)<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mi>x</mi></msub></semantics></math></inline-formula>]<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>2</mn></msub></semantics></math></inline-formula>Cu<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>2</mn></msub></semantics></math></inline-formula>(CN)<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>3</mn></msub></semantics></math></inline-formula> is pressurized. We discovered superconductivity for partial BEDT-STF substitution with <i>x</i> = 0.10–0.12 even at ambient pressure, i.e., a superconducting state is realized in the range between a metal and a Mott insulator without magnetic order. Furthermore, we observed the formation of a superconducting dome by pressurizing the substituted crystals; we assigned this novel behavior to disorder emanating from chemical tuning.