CAP_KILL seems a bit too much privileges for the sole purpose of being able to make ExecReload= work.
Use the + prefix on ExecReload= instead to run "/bin/kill -HUP $MAINPID" with full privileges, ignoring the restrictions from CapabilityBoundingSet=.
See https://www.freedesktop.org/software/systemd/man/systemd.service.html#ExecStart= for further details about the + prefix in ExecReload=.
WantedBy=multi-user.target
[Service]
-ExecReload=/bin/kill -HUP $MAINPID
+ExecReload=+/bin/kill -HUP $MAINPID
ExecStart=@UNBOUND_SBIN_DIR@/unbound -d
NotifyAccess=main
Type=notify
-CapabilityBoundingSet=CAP_IPC_LOCK CAP_NET_BIND_SERVICE CAP_SETGID CAP_SETUID CAP_SYS_CHROOT CAP_SYS_RESOURCE CAP_NET_RAW CAP_KILL
+CapabilityBoundingSet=CAP_IPC_LOCK CAP_NET_BIND_SERVICE CAP_SETGID CAP_SETUID CAP_SYS_CHROOT CAP_SYS_RESOURCE CAP_NET_RAW
MemoryDenyWriteExecute=true
NoNewPrivileges=true
PrivateDevices=true