The Bharatiya Janata Party leader also administered a pledge calling upon students and people to commit themselves to cleanliness.
She later went through the main markets urging shopkeepers and residents to ensure that their town remained clean.
At one point, Hema Malini picked up the broom to demonstrate how people should keep their surroundings tidy.
Along the Yamuna, students from the Bhakti Vedanta Gurukul along with Friends of Vrindavan group spent two hours to pick up trash from the river bank.