Speaking to members from both traditions, the Catholic News Agency reports that he said speaking about reconciliation wasn't enough and reconciliation can only be achieved with action.
He said: "This is the journey that awaits us in the new phase of the dialogue, devoted to reconciliation: we cannot speak of prayer and charity unless together we pray and work for reconciliation and full communion."
The pontiff however commended the value of dialogue between the two groups and said they "are no longer strangers" but rather, through their shared baptism are "members of the household of God".
He went on to say: "We too have been freed from the slavery of estrangement and mutual suspicion."
World Methodist Council: dialogue must reach local level §RV https://t.co/aKJjJz6o7G
— Vatican - news (@news_va_en) October 19, 2017
The members were all in Rome to commemorate the 50th anniversary of the formation of the Joint International Methodist-Catholic Dialogue Commission - the first of which was held in the hill town of Ariccia in Rome on October 1967.
Citing the Second Vatican Council, the pope said that since then, both communities have striven to continue along the path of knowledge and mutual esteem through dialogue that is carried out "in a spirit of honesty and integrity" with "love for the truth, with charity and with humility".
He added: "Now is the time to prepare ourselves, with humble hope and concrete efforts, for that full recognition that will come about, by God's grace, when at last we will be able to join one another in the breaking of the bread.
"So let us advance together, knowing that our journey is blessed by the Lord. It began from him, and it leads to him."
