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No sin is greater than another sin in the eternal sense. All sin separates us from God, and all sin needs to be atoned for. Also, there is no "greatest sin" in the sense of "mortal" and "venial" si...
The greatest sin is not accepting the free gift of eternal life with Jesus Christ when the Holy Spirit offers it to you. This is the only sin that is not forgiven by God, thus giving you a free ride to the Lake of Fire.
I would agree with the responses above, particularly with respect to willful unbelief as being the only unpardonable sin. However, it seems to me that even willful unbelief is caused by a greater "core" sin, which is the sin of pride -- a person's belief that he ultimately has all knowledge, and is also completely without fault in the eyes of God (if he even acknowledges the existence of God), and therefore is not in need of the salvation that God offers in Christ. C.S. Lewis gives a well-reasoned exposition of this viewpoint in a chapter from his book Mere Christianity at the following link: http://www.timesandseasons.org/The_Great_Sin_condensed.pdf
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