Sixty-six advanced heart failure patients referred for CRT with an LV ejection fraction (EF) of < 35% and QRS ≥ 120 ms were studied. We performed equilibrium radionuclide angiography (ERNA) before and 6 mo after CRT. We assessed ventricular dyssynchrony with parameters derived from the first harmonic phase (Ø) analysis of the ERNA time-activity curve and evaluated change in these parameters after 6 mo of CRT. These parameters include novel indices of synchrony (S), a measure of intraventricular contraction order, and entropy (E), a measure of intraventricular contraction disorder, and interventricular synchrony (IVS), a measure of synchronous biventricular function. Forty-seven (71%) patients improved clinically (responders) at 6 mo after CRT whereas 19 (28.8%) showed no change in New York Heart Association class or worsened (nonresponders). The post-CRT changes in QRS duration (P = 0.006), echocardiographic (P = 0.03) and ERNA LVEF (P = 0.0007), LVS (P = 0.004), LVE (P = 0.006), LV standard deviation of ventricular phase (LVSDØ) (P = 0.004), and IVS (P = 0.05) were significantly different between responders and nonresponders. Sixty-two percent of responders had either an LVS < 0.84 or an IVS ≥ 18.8° as opposed to only 16% of nonresponders (P = 0.001). Twenty-nine of 32 (91%) patients with either of these measures responded to CRT (P < 0.01). LVS and IVS are novel measures of LV dyssynchrony derived from ERNA planar analysis. A baseline value of LVS < 0.84 or IVS ≥ 18.8° predicts a positive response to CRT.