AbstractGenuine non‐double‐couple (non‐DC) components of a seismic source, defined here as the non‐DC components that are not due to summation of pure double‐couple (DC) components, provide important insight into special physical processes in non‐earthquake sources such as explosion, volcano eruption and collapse etc. Yet they remain challenging to be resolved. To address the issue and explore the physical mechanism of those special events, we develop a waveform‐polarity‐based moment tensor (WPMT) inversion method and employ it to study physical process in the 2014–2015 Bárðarbunga volcano event sequence. The WPMT method incorporates P‐wave polarity data and seismic waveforms in the source inversion, designs a source simplicity test to check possible complex rupture in the seismic source, and employs a simulated annealing algorithm to search the best source solution. The simplicity test checks consistency of the source processes in the initiation stage of the event and the major energy release process of the event, thus ensuring that the inferred non‐DC components are genuine to the seismic source. Real event and synthetic tests indicate that the WPMT method can identify and resolve genuine non‐DC components in a seismic source. The WPMT inversions of the Bárðarbunga sequence yield many genuine non‐DC source components and reveal that the eruptions are accompanied by seismic activities in depths of 1–5 km with magma migrations out of chambers, collapses of conduits, failures of normal faults, and a magma recharge at a depth of 9 km accompanied by a failure on a nearby normal fault.