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Low-loss (Zn 1- x Ni x )ZrNbTaO 8 (0.02 ≤  x  ≤ 0.10) ceramics possessing single wolframite structure are initiatively synthesized by solid-state route. Based on the results of Rietveld refinement, complex chemical bond theory is used to establish the correlation between structural characteristics and microwave performance in this ceramic system. A small amount of Ni 2+ ( x  = 0.06) in A-site with the fixed substitution of Ta 5+ in B-site can effectually raise the Q  ×  f value of ZnZrNb 2 O 8 ceramic, embodying a dense microstructure and high lattice energy. The dielectric constant and τ f are mainly affected by bond ionicity and the average octahedral distortion. The (Zn 0.94 Ni 0.06 )ZrNbTaO 8 ceramic sample sintered at 1150 °C for 3 h exhibits an outstanding combination of microwave dielectric properties: ε r = 27.88, Q × f  = 128,951 GHz, τ f = –39.9 ppm/°C. Thus, it is considered to be a candidate material for the communication device applications at high frequency. [ABSTRACT FROM AUTHOR]