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In this work, dielectric behavior of CoFe2O4/MWCNT/epoxy nanocomposites affected by concentration, temperature and Au ion irradiation is reported. The CoFe2O4 nanoparticles are synthesized via co‐precipitation technique. The samples of CoFe2O4/MWCNT/epoxy nanocomposites are prepared by varying ferrite contents (upto 50 phr). After that, the dielectric behavior is evaluated using LCR meter. The results exhibited that the dielectric constant of CoFe2O4/MWCNT/epoxy nanocomposites increases with increased ferrite content. The effect of temperature on dielectric of CoFe2O4/MWCNT/epoxy nanocomposites is observed at 27–100°C. The dielectric constant of prepared nanocomposites is gradually enhanced with elevation in temperature up to a certain value then decreased due to accumulation of charges at interfaces. Furthermore, reduced dielectric behavior of prepared nanocomposites can be seen on the account of ion irradiation effect.