<jats:title>Abstract</jats:title><jats:p>Alzheimer's disease (AD) is the most frequent neurodegenerative disorder in the elderly aged over 65. The extracellular accumulation of beta‐amyloid (Aβ) aggregates in the brain is considered as the major event worsening the AD symptoms, but its underlying reason has remained unclear. Here the piezoelectric characteristics of Aβ aggregates are revealed. The vector piezoresponse force microscopy (PFM) analysis results exhibit that Aβ fibrils have spiraling piezoelectric domains along the length and a lateral piezoelectric constant of 44.1 pC N<jats:sup>‐1</jats:sup>. Also, the continuous sideband Kelvin probe force microscopy (KPFM) images display that the increment of charge‐induced surface potential on a single Aβ fibril is allowed to reach above +1700 mV in response to applied forces. These findings shed light on the peculiar mechano‐electrical surface properties of pathological Aβ fibrils that exceed those of normal body components.</jats:p>