Electronic predissociation of CN(B)-Ar-n, (n approximate to 100) clusters has been examined using optical-optical double resonance techniques. Rotationally cold (T-rot approximate to 130 K) CN(A, upsilon=9) fragments were detected following excitation of CN(B,upsilon=0)-Ar-n. An upper bound for the predissociation rate of Gamma(p)<2 x 10(6) s(-1) was determined. These results are consistent with a surface-bound structure for the CN-Ar-n clusters, or a sequential dissociation process that involves a surface-bound intermediate. Demonstration that free CN(A) is produced by predissociation of CN(B)-Ar-n, validates a previous determination of the radiative lifetime for CN(A)7 less than or equal to upsilon less than or equal to 9 levels.