Commentaries:
Barnes' Notes
I will harden - Calamities which do not subdue the heart harden it. In the case of Pharaoh, the hardening was at once a righteous judgment, and a natural result of a long series of oppressions and cruelties.
Other Barnes' Notes entries containing Exodus 4:21:
Exodus 7:13
Exodus 9:7
Acts 2:19
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