Officials also met pastors and attended the inauguration of a humanitarian assistance centre operated by Catholic charity Caritas Aleppo in the Hanano neighbourhood.
The Holy See said: "The delegation was able to meet the Christian communities and their pastors, who expressed their gratitude to the Pope for his constant attention to beloved Syria.
"In addition, he visited Catholic charitable institutions and a number of refugee camps."
The delegation from the Vatican's Dicastery for the Promotion of Integral Human Development included Msgr. Giampietro Dal Toso.
A schedule for the visit, which began last Wednesday and concluded on Monday, also included an ecumenical prayer service coinciding with the week of Prayer for Christian Unity.
A Vatican statement also said: "...the meetings with Catholic charitable entities highlighted the importance of the assistance they provide for the benefit of all the Syrian population.
"With the support of the universal Church and thanks to the generous contribution of the international community, such aid can be intensified in the future to face the growing needs of the people."
The delegation also met with Muslim representatives in the area, to promote the responsibility of faith groups to encourage peace and reconciliation.