Children's Adjustment, Relief, and Education Act or the CARE Act - Amends the Illegal Immigration Reform and Immigrant Responsibility Act of 1996 to repeal the provision prohibiting an unlawful alien's eligibility for higher education benefits based on State residence unless a U.S. national is similarly eligible without regard to such State residence.

Amends the Immigration and Nationality Act to direct the Attorney General to cancel the removal of, and adjust to permanent resident status, certain (inadmissible or deportable) alien secondary or higher education students under the age of 21 with qualifying years of U.S. residency. Amends the Personal Responsibility and Work Opportunity Reconciliation Act of 1996 to make such alien higher education students eligible for education assistance during the pendency of their application for cancellation of removal.