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We report a drastic reduction of hardness of about 61% from WB3 to WB4. The three-dimensional covalent network consisting of boron honeycomb planes interconnected with strong zigzag W-B bonds underlies the high hardness of WB3. Despite the strong intralayer and interstitial B-B bonds, the interlayer B-B nonbonding and the considerably weak zigzag W-B bonding allow the layers of WB4 to cleave readily, which results in the anomalous softening of WB4. The results provide robust evidence that the highest boride of tungsten, which is characterized experimentally by an inexpensive superhard material, should be stoichiometric WB3, not WB4. [ABSTRACT FROM AUTHOR]