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Not sure how late we are to go considering the OP asks for the ‘earliest’ church father’s writings on Mary’s sinlessness but here we go.
Origen
This Virgin Mother of the Only-begotten of God is called Mary, worthy of God, immaculate of the immaculate, one of the one (Homily 1 [A.D. 244]).
Didn't Origen also write this:
(Origen, ca. 240, 'Commentary on The Song of Songs' 3:13, in 'Ancient Christian Writers' 26:237)
"'For all have sinned,' [Romans 3:23] as it is written; and again, as Scripture says: 'There is no just man upon earth that hath done good and hath not sinned;' [Ecclesiastes 7:20] and again: 'No one is free of uncleanness, not even if his life be of but one day.' [Cf. Job 14:4] Therefore Our Lord and Saviour Jesus Christ alone is He 'who did no sin' [cf. 1 Peter 2:22, citing Isaiah 53:9; 2 Corinthians 5:21]"