An analytical approximation of a nonlinear force-free magnetic field (NLFFF) solution was developed in Paper I, while a numerical code that performs fast forward-fitting of this NLFFF approximation to a line-of-sight magnetogram and coronal 3D loops has been described and tested in Paper II. Here we calculate the free magnetic energy E free = E N − E P , i.e., the difference of the magnetic energies between the nonpotential field and the potential field. A second method to estimate the free energy is obtained from the mean misalignment angle change ∆µ = µ P − µ N between the potential and nonpotential field, which scales as E free /E P ≈ tan 2 (∆µ). For four active regions observed with STEREO in 2007 we find free energies in the range of q free = (E free /E P ) ≈ 1% − 10%, with an uncertainty of less than ±2% between the two methods, while the free energies obtained from 11 other NLFFF codes exhibit a larger scatter of order ≈ ±10%. We find also a correlation between the free magnetic energy and the GOES flux of the largest flare that occurred during the observing period, which can be quantified by an exponential relationship, F GOES ∝ exp (q free /0.015), implying an exponentiation of the dissipated currents.