The output power of piezoelectric energy harvester (PEH) at the resonance frequency is dependent on the electromechanical coupling factor (
k
p
) of the piezoceramic, which is proportional to
d
33
/
ε
T
33
1
/
2
, where
d
33
and
ε
T
33
are the piezoelectric change and dielectric constants, respectively. Therefore, the piezoceramic for the PEH should have a large
d
33
and a small
ε
T
33
. [001]-texturing can be used for developing piezoceramics for PEH because it generally increases
d
33
without increasing
ε
T
33
. The 0.96(K0.5Na0.5)(N1-zSz)O3-0.03(Bi0.5Ag0.5)ZrO3-0.01SrZrO3 [KN(N1-zSz)-BAZ-SZ] piezoceramics were textured along the [001] orientation, and the piezoceramic (
z
=
0.01
) showed a large
k
p
of 0.77, which is the largest
k
p
for KNN-related piezoceramics reported in the literature. The cantilever-type PEH manufactured using the KN(N0.99S0.01)-BAZ-SZ piezoceramic exhibited a large output power density of 7.86 mW/cm3 at resonance frequency because of its large
k
p
. To date, this is the largest power density for PEHs manufactured utilizing lead-free piezoceramics. Hence, the [001]-textured KN(N0.99S0.01)-BAZ-SZ piezoceramic is an excellent candidate for PEH, and [001]-texturing is a very efficient method for developing piezoceramics for PEH.