Stroke is often caused by carotid plaque rupture, with rupture potential indicated by plaque structure and composition. Delineating carotid plaque components that confer rupture risk is vital to stoke prevention. We have previously shown that ARFI Log Variance of Acceleration, log(VoA), discriminates intraplaque hemorrhage (IPH) from lipid-rich necrotic core (LRNC) and collagen (COL) from calcium (CAL) in vivo in humans, while ARFI peak displacement does not. We hypothesize that log(VoA) performance will be further improved by harmonic tracking of ARF-induced displacement. In a pilot clinical study of six carotid plaques imaged in vivo in patients undergoing carotid endarterectomy (CEA), plaque component contrast-to-noise ratio (CNR) achieved by harmonic log(VoA) was compared to that achieved by tracking at fundamental low (4.0 MHz, FL) and high (8.89 MHz, FH) frequencies with validation by spatially-matched histology derived from the extracted plaque specimens. Over all examined plaques, harmonic and both fundamental low and high log(VoA) distributions statistically differentiated plaque components (Wilcoxon, mathrm{p} < 0.01, panel iv). Harmonic log(VoA) achieved the highest CNR between COL and LRNC, which is relevant to fibrous cap delineation, but FH tracking yielded the highest CNR between LRNC and IPH and between COL and CAL. These results suggest that combined harmonic and FH tracking could improve ARFI log(VoA) characterization of carotid plaque components that are correlated to rupture.