This paper reports the structural, morphological, spectroscopic, dielectric, ac conductivity, and impedance properties of nanocrystalline Mn
1-x
Zn
x
Fe
2
O
4
. The nanocrystalline Mn–Zn ferrites were synthesized using a solvent-free combustion reaction method. The structural analysis using X-ray diffraction (XRD) pattern reveals the single-phase of all the samples and the Rietveld refined XRD patterns confirmed the cubic-spinel structure. The calculated crystallite size values increase from 8.5 nm to 19.6 nm with the Zn concentration. The surface morphological analysis using field emission scanning electron microscopy and the transmission electron microscopy confirms the nano size of the prepared ferrites. X-ray photoelectron spectroscopy was used to study the ionic state of the atoms present in the samples. Further, the high-resolution Mn 2p, Zn 2p, Fe 2p, and O 1s spectra of Mn
1-x
Zn
x
Fe
2
O
4
does not result in the appearance of new peaks with Zn content, indicating that the Zn substitution does not change the ionic state of Mn, Zn, Fe, and O present in nanocrystalline Mn
1-x
Zn
x
Fe
2
O
4
. The investigated electrical properties show that the dielectric constant, tan δ and ac conductivity gradually decrease with increasing Zn substitution and the sample Mn
0
·
2
Zn
0
·
8
Fe
2
O
4
has the lowest value of conductivity at 303 K. The ac conductivity measured at different temperatures shows the semiconducting nature of the ferrites. The impedance spectra analysis shows that the contribution of grain boundary is higher compared with the grain to the resistance. The obtained results suggest that the Zn substituted manganese ferrite nanoparticles can act as a promising candidate for high-frequency electronic devices applications.