On 4 January 2003 Longley was appointed Auxiliary Bishop of Westminster and Titular Bishop of Zarna by Pope John Paul II. He said he was "greatly honoured" and "very much overwhelmed" by his appointment. Longley received his episcopal consecration on the following 24 January from Cardinal Cormac Murphy-O'Connor, with Bishops Arthur Roche and Kieran Conry serving as co-consecrators. In 2007, Longley played a prominent role in the integration of the independent Soho Masses Pastoral Council, a group that sponsors Masses for homosexual Catholics, into the Archdiocese. The Bishop helped to form an agreement that moved the group's liturgies from an Anglican parish to a Catholic church, as well as a statement on ministry to homosexual Catholics that, while following Catholic teaching on homosexuality, underscored that "the Church's pastoral outreach recognises that baptised persons with a homosexual inclination continue to look to the Church for a place where they might live in authentic human integrity and holiness of life." In a BBC interview, Longley said that "it's never been the practice of the Catholic Church, as it were, to 'means-test' people before admitting them to the celebration of the Eucharist. It would be a mistake to jump to conclusions or to generalise about anybody's particular lifestyle, or their state of grace." Longley is the head of the Diocesan Pastoral Board and has responsibilities for the Deaneries of Camden, Hackney, Islington, Marylebone, Tower Hamlets, and Westminster. He is considered to be a conservative who is "friendly" to the traditional Latin Mass, but also a "born diplomat." His name was mentioned as a possible successor to Cardinal Murphy-O'Connor as Archbishop of Westminster and thus often considered to be the 'head' of the Church in England and Wales, but the position ultimately went to Archbishop Vincent Nichols.
Archbishop of Birmingham
On 1 October 2009, Pope Benedict XVI appointed Bishop Longley as the Archbishop of Birmingham. He succeeds Archbishop Vincent Nichols, who was translated from Birmingham to Westminster earlier in 2009. Archbishop Longley was installed at St Chad's Cathedral on 8 December 2009, the feast of the Immaculate Conception. Before the ceremony, Archbishop Longley spoke of how much he was looking forward to joining both the Catholic and wider Christian communities in the Midlands and contributing to their work. Archbishop Longley played a leading role in the plans for the beatification of Cardinal John Henry Newman and presented the petition for canonisation to Pope Benedict XVI, which took place in Cofton Park, Birmingham on 19 September 2010 during the papal visit to the United Kingdom in September 2010. On 5 January 2011, Archbishop Longley was appointed among the first members of the newly created Pontifical Council for the Promotion of the New Evangelisation. Archbishop Longley is also co-Chair of ARCC and has previously served as Moderator of the Steering Committee of Churches Together in Britain and Ireland, as well as Assistant General Secretary of Catholic Bishops' Conference of England and Wales with responsibilities for Ecumenism and Interfaith Affairs. On Tuesday, 18 September 2012, Pope Benedict XVI named Archbishop Longley to serve as one of the Synod Fathers for the October 2012 13th Ordinary General Assembly of the Synod of Bishops on the New Evangelization.