Archbishop of Westminster Cardinal Vincent Nichols branded the announcement to cap the number of unaccompanied youngsters being allowed into Britain under the Dubs amendment at 350 as "truly shocking".
He said: "By repealing Article 67 of the Immigration Act 2016, known as the Dubs amendment, the Government is seen by many as abandoning its statutory and moral duty to take effective action for the protection of vulnerable, unaccompanied child refugees.
"If this is the case, then it is truly shocking."
I ask the Home Secretary to review urgently the decision to repeal Art 67 and to honour the original intention behind the Dubs Amendment.
— Cardinal Nichols (@CardinalNichols) February 12, 2017
Politicians and campaigners originally called for 3,000 children to be transferred under the Dubs scheme, the brainchild of Labour peer and former refugee Lord Alf Dubs.
The government said more than 900 children were resettled in the UK last year, either under the Dubs amendment, or the Dublin Regulation which protects those with family links in the country.
Cardinal Nichols also said: "The Home Office have stated that during 2016 over 900 unaccompanied children were brought to safety from Europe, including 750 from Calais.
"However, the need is evidently far greater and I am informed that there are a number of Local Authorities willing and resourced to take many more of these children into their care.
"I urge the Government to look again at all available resources and to work with renewed vigour, internationally and at home, to support and enable programmes to assist these vulnerable children."
Those concerned about the government repealing Article 67 of the Immigration Act 2016 were also encouraged by the Catholic leader to come forward to take in refugees.
Cardinal Nichols joins high-profile figures including the Archbishop of Canterbury Rt Rev Justin Welby to criticise the government's decision on the lone child refugee scheme.
Meanwhile, faith leaders, children and local politicians joined Lord Dubs on Saturday to deliver a petition signed by 50,000 people accusing the Government of a "very shabby cop out".