The kinetics of elementary reactions involved in the chain chlorination of cyclopropane are examined using a combination of absolute and relative rate constant measurements and first principles electronic structure calculations. Relative rate methods are used in a smog chamber FTIR apparatus to determine k(Cl + C-C3H6) = (1.15 +/- 0.17) x 10(-13) and k(Cl + C-C3H5Cl) = (1.06 +/- 0.18) x 10(-12) cm(3) molecule(-1) s(-1) in 10-700 Torr of air, or N-2, diluent at 296 K. Absolute rate coefficients for the reaction of Cl with cyclopropane are measured between 293 and 623 K by a laser-photolysis/CW infrared absorption method. The data can be represented in Arrhenius form as k(Cl + C-C3H6) = ((1.8 +/- 0.3) x 10(-10) cm(3) molecule(-1) s(-1))e(-(2150+/-100)/T). To support the experimental investigations, first principles electronic structure calculations are performed. Vibrational spectra Of C-C3H5Cl, C-C3H4O2, and C-C3H3Cl3 are calculated and are presented. gem-C3H4O2 is calculated to be the kinetically and thermodynamically most favored dichlorocyclopropane. The experimental observations are consistent with the computational findings.